Stoten D 18 07582R1

Elsevier Editorial System(tm) for Science of
the Total Environment

Manuscript Draft
Manuscript Number: STOTEN-D-18-07582R1
Title: Impact of Mg Rich Synthetic Gypsum Application on the Environment

and Palm Oil Quality
Article Type: Research Paper
Keywords: cytotoxic; heavy metals; kieserite; magnesium; rare earth

element
Corresponding Author: Dr. Che Fauziah Ishak, Ph.D.
Corresponding Author's Institution:
First Author: Sahibin Abd Rahim, PhD
Order of Authors: Sahibin Abd Rahim, PhD; Shamshuddin Jusop, PhD; Che
Fauziah Ishak, Ph.D.; Radziah Othman, PhD; Wan Mohd Razi Idris, PhD; Enio
Mohd Sufian Kang, PhD
Abstract: A study was conducted in an oil palm plantation in Peninsular

Malaysia to elucidate the effects of applying Magnesium Rich Synthetic
Gypsum (MRSG), a by-product of chemical plant, on the chemical properties
of soil, the uptake of heavy metals by the palm trees, the oil quality
and its impact on the surrounding environment. The results showed that
MRSG application onto soil cropped to oil palm could bring positive
impact in terms of soil chemical properties and oil palm production. The
quality of the oil was not significantly affected by the continuous MRSG
application as shown by the low heavy metals and trace elements of
concern content (Cu: 0.062 mg/kg; Fe: 2.10 mg/kg; Mn: 1.93 mg/kg; Pb:
0.006 mg/kg; Zn: 0.103 mg/kg; Cr: 0.354 mg/kg; Ni: 0.037 mg/kg). From the
I-geochem index, the soil was found to have values ranging from -3.81 to
-1.03 which is considered as uncontaminated. Further, its application did
not result in negative impact on the surrounding environment; hence, the
quality of the soil and surface water in the plantation and/or the
surrounding area remained intact. Phytotoxic elements in the oil palm
tissue (As: 0.12 mg/kg; Se: 0.05 mg/kg; Zn: 1.48 mg/kg; Ce: 0.47 mg/kg;
La: 0.26 mg/kg; Sr: 3.03 mg/kg) and cytotoxic elements in the oil were
below the acceptable limit. Based on the results of the Environmental
Monitoring out during the period of the study, it was concluded that
application of the by-product of the chemical plant as a source of Mg to
enhance soil fertility in the oil palm plantation was considered safe and
sustainable. The effects of applying MRSG and Chinese kieserite was
almost similar. So, MRSG can be used as a possible source of Mg to
replace Chinese kieserite for oil palm production on the Ultisols in
Peninsular Malaysia.
Response to Reviewers: Abstract: To rewrite again, please avoid to repeat

sentences or expressions.
Response to Reviewer comment: The abstract has been rewritten and
repeated sentences has been removed accordingly.
Graphical abstract: Personally I consider that is a lack of respect (to
your future readers) to send a graphic like this one. Please, improve the
quality and specially the description: the brown and black circle is a
fruit? The triangles represent the MRSG uptake by plant? Use labels,
arrows
Response to Reviewer comment: The graphical abstract has been improved.
Line 44: "Malaysia has currently more than 5 million ha cultivated with
oil palm
Response to Reviewer comment: Has been improved accordingly.
Line 53: delete "The" at the beginning of the sentence

Line 54:…..presence "of "Al3+

Lines 56-59: repetitive, please rephrase

Response to Reviewer comment:Has been rephrased accordingly.
Line 65: add "elements" after rare earth, "produces" instead of "is
producing"
Response to Reviewer comment:Has been improved accordingly.
Line 68. Add the reference/year

Response to Reviewer comment: Has been added.
Line 73: to rephrase! It's the same as line 72

Response to Reviewer comment:Repeated sentence has been removed.
Line 75: replace "quantity" by "amount"

Response to Reviewer comment: Has been replaced accordingly.
Line79: to rephrase! It's the same as line 75

Response to Reviewer comment:Has been rephrased accordingly.
Lines 83-84: not clear. If the concentration of rare elements compounds

are below 1% why are they included in the concern list? Based on what?
Response to Reviewer comment: The reason is La and Ce are cytotoxic

elements. This sentence has been inserted in the paragraph.
Lines 90-93:
aims instead of objectives,
1) "to characterize the soil", in terms of what?
2) "on the surrounding environment", be clearer
3) "its oil quality" instead of "the quality of its soil"
Response to Reviewer comment: Has been improved according to suggestion.
In my opinion is better to start with the description of the study area

(plus experimental site), then talk about the sampling (soils, surface
water, palm tissues, palm oil), soil properties, determination of heavy
metals and others (in subsections, maybe separated by matrix?) and
finally pollution indexes. I would also include all application details
(ex. Dates) in Table 1.
Response to Reviewer comment: Has been improved according to suggestion.
Lines 100-102: please rephrased? …its elemental composition was
determined by ICP-OES using aqua regia solution, how many gr of sample
were used?
Response to Reviewer comment: The weight of sample has been stated.
Lines 104-109: rephrased. Delete the last part: "the current paper
concentrates (by the way, is focus, not concentrates) only on
explaining……..", we already know what is the aim of your paper, no need
to explain it again.
Response to Reviewer comment: The sentence has been deleted.
Lines 111-114: what was the criteria to choose the "appropriate

location"? As you might know, soil properties and composition can be
highly variable within the same study area.
Lines 123-130:
define "GML"
how many oil palms were collected within each experimental plot?
Response to Reviewer comment: Has been improved. GML has been defined in
section 1.0. Number of palms in an experimental plot has been stated.
Line 127-128: delete "it was followed by" and replace by "The rest of the
application took place"
Response to Reviewer comment: This paragraph has been reconstructed to
follow the flow suggested.
Lines 129-130: repetitive…..-baseline data- and -reference information-
Response to Reviewer comment: Repetation has been removed.
Line 133: why from frond 17? Explain it.

Response to Reviewer comment: Reason has been explained.
Lines 133-134: what "appropriate times and locations" means? Is very

subjective. Be clearer or complete information given in Table 1.
Response to Reviewer comment: Information has been given in table.
Lines 138-140: not clear, please explain it better

Lines 144-145: "Topsoils from all experimental blocks were sampled and
analyzed to get the baseline data before applying the treatments".
Response to Reviewer comment: Has been improved.
Lines 150-154: what about water properties (like pH)? I would consider it
within the "water baseline data", how do you perform the sampling? Water
were collected on which type of bottles? Were they stored? Acidified?
Immediately analyzed for heavy metals concentration?
Lines 161-165: again, there is no details about the sampling itself.
Line 174: define "OER"

Response to Reviewer comment: Has been defined.
Line 179: pipette method? Add a reference please. Replace: "The clay
fraction of the topsoil was X-rayed" by "was determined by Xray".
Response to Reviewer comment:Has been improved.
Lines 191-197: how many gr of soil were weighted?. The samples were
digested on hotplate or microwave? What about certified reference
materials, recoveries for each metal, number of blanks for each batch of
samples, number of replicates if it's the case?. Without this information
you can't validate your data! It's crucial information that must be
included.
Lines 199-231: include number of equation within the text and also at the
beginning of each one. What is the Bn value? Response to Reviewer
comment: Has been included.
Line 215: " a factor of"

Lines 218-223: not clear, rephrase.

Lines 234-243: same problem describe for the section 2.10 (Lines 191-
197).
Lines 253-256: not clear and repetitive "the elements present….were

identified by FESEM-EDX" and then again "The elemental composition of
….determined by the FESEM-EDX"…."were at best a semi-quantitative
measurement", do you mean that is the best method to semi-quantify the
elemental composition?
Response to Reviewer comment: Has been improved accordingly. Repetation
has been deleted.
Lines 257-261: repetitive first you write "…detailed elemental

composition of…..Table 2" and then again "the concentration of heavy
metals…..is shown in Table 2".
Line 261: define SIRIM and DOA.

Response to Reviewer comment: Has been defined accordingly.
Lines 263-264: in my opinion, Cd concentration is not that low. The

accumulation of heavy metals from MRSG depends also on the application
rates. Have you considered this parameter?. What about rare elements?
They mention earlier that these elements are also of concern. What about
other toxic heavy metals (such as Cr, Co or Ni)?
Response to Reviewer comment: In this project, MRSG is used as a source
of Mg. So the rate is reflecting the amount of Mg needed in the soil. Mg
is needed in a small amount in the field, so the concentration of TEOC is
not that high.
Section 3.2: instead of describing soil colors it would be better to

discuss more about mineral soil composition and how it affects the
physicochemical properties.
Lines 292-295: I think that table 3 must be cited here. You mention that
topsoil pH was 4.9, is this a mean value?, if yes, you have to include
SD. And where are the data of topsoils? you should include them.
Response to Reviewer comment: Has been improved accordingly
Lines 309-310: the whole sentence doesn't make sense.

Response to Reviewer comment: The sentences has been removed.
Lines 334-336: define what a "soil investigation level" is.

Response to Reviewer comment: Has been defined accordingly.
Lines 343-346: in the table you must show the difference between control
1 and control 2, if not it's impossible to know when you're talking about
kieserite or GML application. Response to Reviewer comment: Has been
improved accordingly.
Lines 348-356: more references about rare elements has to be included.

Are the Chinese and Sweden soil studies the same? They have the same
reference, if not please add it.
Response to Reviewer comment:We couldnt find the literature relating to
this.
Lines 365-370: how can you affirm that there is a positive impact on Mg,
Ca and S content in soils if you only have considered the baseline data,
shown in Table 3? Have you measured the concentration of these elements
after treatment?
Response to Reviewer comment: This paper focuses more on TEOC and HM.
Other elements have been discussed in earlier paper.
Line 377: is Th a harmful element?

Response to Reviewer comment: Yes. It is slightly radioactive. But the
level is too low and cannot be detected in the surface water, oil and
soil.
Lines 387-392: this sentence looks more like a final conclusion.

Response to Reviewer comment: Sentences have been removed.
Line 401: "palm oil safe limit" compared to what? Literature or

regulations?
"Highly appreciated?" Personally I would use constructions like: the

authors would like to thank, we also want to express our gratitude, we
want to thank……
Table 1: I would include more info, for example dates (see my comments
above).
Table 2: what does "trace" mean? you must include limits of detection or
quantification. Ppm is for mg/kg of dry sample? Response to Reviewer
comment: Has been improved.
Table 4: there is a typing error (I guess) it's B (for Boron) and not Bo!
Response to Reviewer comment: Has been corrected.
Table 5: "not detected", the same problem as "trace", see my comment
above. Please include a mark to make the difference between control 1 and
2.
Table 9: concentrations for As are 0? How is that possible? Response

to Reviewer comment:Has been improved.
Table 10: why not compare the results with European regulations about
trace metals in food or with the FAO/WHO Codex Alimentarius? If they are
available of course.
Response to Reviewer comment:Has been inserted.
Figure 1: for me this figure is pointless.

Response to Reviewer comment:Figure has been removed.
Figure 2: include GPS points within the map

Response to Reviewer comment:GPS has been included
Figure 3: typing error, block 2 (next to block 3) should be block 4.

Cover Letter
Title Page
Impact of Mg Rich Synthetic Gypsum Application on the Environment and Palm Oil
1 Quality
2
3 Sahibin Abd Rahima, Shamshuddin Jusopb, Che Fauziah Ishakb*, Radziah Othmanb, Wan
4
5 Mohd Razi Idrisc and Enio Mohd Sufian Kangd
6
7
8 a
9 Environmental Science Program, Faculty of Science and Natural Resources, Universiti
10 Malaysia Sabah, 88400 Kota Kinabalu, Sabah, Malaysia
11 haiyan@ukm.edu.my
12
13 b
14
Department of Land Management, Faculty of Agriculture, Universiti Putra Malaysia, 43400
15 Serdang, Selangor, Malaysia
16 shamshud@upm.edu.my; cfauziah@upm.edu.my; radziah@upm.edu.my
17
18 c
School of Environmental and Natural Resources Sciences, Faculty of Science and
19
20 Technology, Universiti Kebangsaan Malaysia, 43600 Bangi, Selangor, Malaysia
21 razi@ukm.edu.my
22
23 d
Department of Science and Technical Education, Faculty of Educational Studies, Universiti
24
25
Putra Malaysia, 43400 Serdang, Selangor, Malaysia
26 enio@upm.edu.my
27
28 *Correspondence: cfauziah@upm.edu.my; Tel: +603-8947 4938
29
30
31
32
33
34
35
36
37
38
39
40
41
42
43
44
45
46
47
48
49
50
51
52
53
54
55
56
57
58
59
60
61
62
63
64
65
*Responses to Reviewers Comments
Comments Rebuttal
Abstract: To rewrite again, please avoid to repeat The abstract has been rewritten
sentences or expressions. and repeated sentences has been
removed accordingly.
Graphical abstract: Personally I consider that is a lack of The graphical abstract has been
respect (to your future readers) to send a graphic like this improved.
one. Please, improve the quality and specially the
description: the brown and black circle is a fruit? The
triangles represent the MRSG uptake by plant? Use
labels, arrows
Line 44: "Malaysia has currently more than 5 million ha Has been improved accordingly.
cultivated with oil palm
Line 53: delete "The" at the beginning of the sentence Has been improved accordingly.
Line 54:…..presence "of "Al3+ Has been improved accordingly.
Lines 56-59: repetitive, please rephrase Has been rephrased accordingly.
Line 65: add "elements" after rare earth, "produces" Has been improved accordingly.
instead of "is producing"
Line 68. Add the reference/year Has been added.
Line 73: to rephrase! It's the same as line 72 Repeated sentence has been
removed.
Line 75: replace "quantity" by "amount" Has been replaced accordingly.
Line79: to rephrase! It's the same as line 75 Has been rephrased accordingly.
Lines 83-84: not clear. If the concentration of rare The reason is La and Ce are
elements compounds are below 1% why are they cytotoxic elements. This sentence
included in the concern list? Based on what? has been inserted in the
paragraph.
Lines 90-93: Has been improved according to
aims instead of objectives, suggestion.
1) "to characterize the soil", in terms of what?
2) "on the surrounding environment", be clearer
3) "its oil quality" instead of "the quality of its soil"
In my opinion is better to start with the description of the Has been improved according to
study area (plus experimental site), then talk about the suggestion.
sampling (soils, surface water, palm tissues, palm oil),
soil properties, determination of heavy metals and others
(in subsections, maybe separated by matrix?) and finally
pollution indexes. I would also include all application
details (ex. Dates) in Table 1.
Lines 100-102: please rephrased? …its elemental The weight of sample has been
composition was determined by ICP-OES using aqua stated.
regia solution, how many gr of sample were used?
Lines 104-109: rephrased. Delete the last part: "the The sentence has been deleted.
current paper concentrates (by the way, is focus, not
concentrates) only on explaining……..", we already
know what is the aim of your paper, no need to explain it
again.
Lines 111-114: what was the criteria to choose the Has been improved accordingly.
"appropriate location"? As you might know, soil
properties and composition can be highly variable within
the same study area.
Lines 123-130: Has been improved. GML has
define "GML" been defined in section 1.0.
how many oil palms were collected within each Number of palms in an
experimental plot? experimental plot has been stated.
Line 127-128: delete "it was followed by" and replace by This paragraph has been
"The rest of the application took place" reconstructed to follow the flow
suggested.
Lines 129-130: repetitive…..-baseline data- and - Repetation has been removed.
reference information-
Line 133: why from frond 17? Explain it. Reason has been explained.
Lines 133-134: what "appropriate times and locations" Information has been given in
means? Is very subjective. Be clearer or complete table.
information given in Table 1.
Lines 138-140: not clear, please explain it better Has been improved accordingly.
Lines 144-145: "Topsoils from all experimental blocks Has been improved.
were sampled and analyzed to get the baseline data
before applying the treatments".
Lines 150-154: what about water properties (like pH)? I Has been improved accordingly.
would consider it within the "water baseline data", how
do you perform the sampling? Water were collected on
which type of bottles? Were they stored? Acidified?
Immediately analyzed for heavy metals concentration?
Lines 161-165: again, there is no details about the Has been improved accordingly.
sampling itself.
Has been defined.
Line 174: define "OER"
Line 179: pipette method? Add a reference please. Has been improved.
Replace: "The clay fraction of the topsoil was X-rayed"
by "was determined by Xray".
Lines 191-197: how many gr of soil were weighted?. The Has been improved.
samples were digested on hotplate or microwave? What
about certified reference materials, recoveries for each
metal, number of blanks for each batch of samples,
number of replicates if it's the case?. Without this
information you can't validate your data! It's crucial
information that must be included.
Lines 199-231: include number of equation within the Has been included.
text and also at the beginning of each one. What is the Bn
value?
Line 215: " a factor of" Has been improved.
Lines 218-223: not clear, rephrase. Has been improved accordingly.
Lines 234-243: same problem describe for the section Has been improved.
2.10 (Lines 191-197).
Lines 253-256: not clear and repetitive "the elements Has been improved accordingly.
present….were identified by FESEM-EDX" and then Repetation has been deleted.
again "The elemental composition of ….determined by
the FESEM-EDX"…."were at best a semi-quantitative
measurement", do you mean that is the best method to
semi-quantify the elemental composition?
Lines 257-261: repetitive first you write "…detailed Has been improved accordingly.
elemental composition of…..Table 2" and then again "the
concentration of heavy metals…..is shown in Table 2".
Line 261: define SIRIM and DOA. Has been defined accordingly.
Lines 263-264: in my opinion, Cd concentration is not In this project, MRSG is used as a
that low. The accumulation of heavy metals from MRSG source of Mg. So the rate is
depends also on the application rates. Have you reflecting the amount of Mg
considered this parameter?. What about rare elements? needed in the soil. Mg is needed
They mention earlier that these elements are also of in a small amount in the field, so
concern. What about other toxic heavy metals (such as the concentration of TEOC is not
Cr, Co or Ni)? that high.
Section 3.2: instead of describing soil colors it would be Has been improved accordingly.
better to discuss more about mineral soil composition and
how it affects the physicochemical properties.
Lines 292-295: I think that table 3 must be cited here. Has been improved accordingly
You mention that topsoil pH was 4.9, is this a mean
value?, if yes, you have to include SD. And where are the
data of topsoils? you should include them.
Lines 309-310: the whole sentence doesn't make sense. The sentences has been removed.
Lines 334-336: define what a "soil investigation level" is. Has been defined accordingly.
Lines 343-346: in the table you must show the difference Has been improved accordingly.
between control 1 and control 2, if not it's impossible to
know when you're talking about kieserite or GML
application.
Lines 348-356: more references about rare elements has We couldnt find the literature
to be included. Are the Chinese and Sweden soil studies relating to this.
the same? They have the same reference, if not please
add it.
Lines 365-370: how can you affirm that there is a This paper focuses more on
positive impact on Mg, Ca and S content in soils if you TEOC and HM. Other elements
only have considered the baseline data, shown in Table have been discussed in earlier
3? Have you measured the concentration of these paper.
elements after treatment?
Line 377: is Th a harmful element? Yes. It is slightly radioactive. But

the level is too low and cannot be
detected in the surface water, oil
and soil.
Lines 387-392: this sentence looks more like a final Sentences have been removed.
conclusion.
Line 401: "palm oil safe limit" compared to what? Has been improved.
Literature or regulations?
"Highly appreciated?" Personally I would use Has been improved.
constructions like: the authors would like to thank, we
also want to express our gratitude, we want to thank……
Table 1: I would include more info, for example dates Has been improved.
(see my comments above).
Table 2: what does "trace" mean? you must include limits Has been improved.
of detection or quantification. Ppm is for mg/kg of dry
sample?
Table 4: there is a typing error (I guess) it's B (for Boron) Has been corrected.
and not Bo!
Table 5: "not detected", the same problem as "trace", see Has been improved.
my comment above. Please include a mark to make the
difference between control 1 and 2.
Table 9: concentrations for As are 0? How is that Has been improved.
possible?
Table 10: why not compare the results with European Has been inserted.
regulations about trace metals in food or with the
FAO/WHO Codex Alimentarius? If they are available of
course.
Figure 1: for me this figure is pointless. Figure has been removed.
Figure 2: include GPS points within the map GPS has been included
Figure 3: typing error, block 2 (next to block 3) should be Has been improved.
block 4.
*Revised manuscript with changes marked
Click here to view linked References
1 Impact of Mg Rich Synthetic Gypsum Application on the Environment and Palm Oil
2 Quality
3
4 Sahibin1, A. R., J. Shamshuddin2, C.I. Fauziah2*, O. Radziah2, I. Wan Mohd Razi3 and M.S.K.
5 Enio4
6
1
7 Environmental Science Program, Faculty of Science and Natural Resources, Universiti Malaysia
8 Sabah, 88400 Kota Kinabalu, Sabah, Malaysia
9
2
10 Department of Land Management, Faculty of Agriculture, Universiti Putra Malaysia, 43400
12
3
13 School of Environmental and Natural Resources Sciences, Faculty of Science and Technology,
14 Universiti Kebangsaan Malaysia, 43600 Bangi, Selangor, Malaysia
15
4
16 Department of Science and Technical Education, Faculty of Educational Studies, Universiti
17 Putra Malaysia, 43400 Serdang, Selangor, Malaysia
18
*
19 Correspondence: cfauziah@upm.edu.my; Tel: +603-8947 4938
20
21 Abstract
22 A study was conducted in an oil palm plantation in Peninsular Malaysia to elucidate the effects
23 of applying Magnesium Rich Synthetic Gypsum (MRSG), a by-product of chemical plant, on the
24 chemical properties of soil, the uptake of heavy metals by the palm trees, the oil quality and its
25 impact on the surrounding environment. The results showed that MRSG application onto soil
26 cropped to oil palm could bring positive impact in terms of soil chemical properties and oil palm
27 production. The quality of the oil was not significantly affected by the continuous MRSG
28 application as shown by the low heavy metals and trace elements of concern content (Cu: 0.062
29 mg/kg; Fe: 2.10 mg/kg; Mn: 1.93 mg/kg; Pb: 0.006 mg/kg; Zn: 0.103 mg/kg; Cr: 0.354 mg/kg;
30 Ni: 0.037 mg/kg). From the I-geochem index, the soil was found to have values ranging from -
31 3.81 to -1.03 which is considered as uncontaminated. Further, its application did not result in
32 negative impact on the surrounding environment; hence, the quality of the soil and surface water
Open
1
33 in the plantation and/or the surrounding area remained intact. Phytotoxic elements in the oil palm
34 tissue (As: 0.12 mg/kg; Se: 0.05 mg/kg; Zn: 1.48 mg/kg; Ce: 0.47 mg/kg; La: 0.26 mg/kg; Sr:
35 3.03 mg/kg) and cytotoxic elements in the oil were below the acceptable limit. Based on the
36 results of the Environmental Monitoring out during the period of the study, it was concluded that
37 application of the by-product of the chemical plant as a source of Mg to enhance soil fertility in
38 the oil palm plantation was considered safe and sustainable. The effects of applying MRSG and
39 Chinese kieserite was almost similar. So, MRSG can be used as a possible source of Mg to
40 replace Chinese kieserite for oil palm production on the Ultisols in Peninsular Malaysia.
41 Keywords: cytotoxic; heavy metals; kieserite; magnesium; rare earth element
42
43 1.0 Introduction
44 Over the last few decades, the main sources of magnesium fertilizer for oil palm plantation in
45 Malaysia are kieserite from Germany and ground magnesium limestone (GML) which is locally
46 mined. Synthetic magnesium sulphate from China (Chinese kieserite) has also made some in
47 road since the late 1990’s although its scale of use is significantly less than the two fertilizers
48 stated earlier.
49
50 The high price of Germany kieserite and low reactivity of GML make it feasible for the
51 plantation industry to seek for an alternative source of magnesium fertilizer. The chemical plant
52 in Malaysia that extract rare earth elements produces a by-product called Neutralization
53 Underflow (NUF) residue. This material, also called Mg Rich Synthetic Gypsum (MRSG), can
54 be applied in oil palm plantations as a source of Mg fertilizer. The MRSG is classified as
55 Scheduled Waste (SW205) by the Department of Environment (DoE), Ministry of Natural
Open
2
56 Resources and Environment, Malaysia (DOE, 1974). The Atomic Energy Licensing Board
57 (AELB, 2008) of Malaysia had confirmed that MRSG was non-radioactive. It means that the
58 material has the potential to be utilized in agriculture. It is therefore worthwhile to determine if
59 this MRSG can replace the imported kieserite as Mg source to sustain oil palm growth and palm
60 oil production in the long run. Since this by-product contains some trace elements of concern
61 (TEOC) (As, Cd, Se, Zn, Ce, La and Sr), so its impact on the environment needs to be evaluated
62 before it can be recommended for application. However, there were several studies that showed
63 very little accumulation of heavy metals in upper plant biomass of oil crops as reported by
64 Violina et al. (2005); Sengalevitch (1999); Szyczewski et al. (2016) and Tyler (2004).
65
66 Malaysia has currently more than 5 million ha cultivated with oil palm, which constitutes the
67 biggest arable land area allocated to agriculture in the country. Soils in Peninsular Malaysia used
68 for growing oil palm are Ultisols, dominated by kaolinite, gibbsite, goethite and hematite in the
69 clay fraction (Shamshuddin and Ismail, 1995; Shamshuddin and Fauziah, 2010). According to
70 Shamshuddin et al. (1991), the cation exchange capacity (CEC) of Ultisols was low, resulting in
71 low retention in the soil and thus low availability of Mg and Ca that limits crop productivity.
72 With low pH, Al3+ is present in amount that affects the growth oil palm roots.
73
74 Oil palm productivity is limited by the infertile nature of the soils; hence, fertilizer application
75 become an important issue to sustain production. Ultisols usually have plant nutrients
76 insufficient for normal production, unless they are adequately fertilized. About 60% of the cost
77 of palm oil production comes from fertilizer that requires to supply the needed nutrients.
Open
3
78 Ca, Mg and S are needed by oil palm under production in high amount for its healthy growth
79 and/or production, and it is believed that these macronutrients can be added into soils in the
80 plantations by continuous application of MRSG. Besides, by virtue of being alkaline (the pH of
81 MRSG is 8.8), due to the presence of magnesium hydroxide, calcium hydroxide and some
82 calcium carbonate, soil pH can be raised to the desired level for oil palm cultivation.
83 Furthermore, MRSG contained some Si that may help prevent certain oil palm disease prevailing
84 in the plantations throughout the country (Najihah et al., 2014).
85
86 Components of MRSG include rare earth compounds lanthanum (La) and cerium (Ce); both
87 were present at about 1 %. However, La and Ce are cytotoxic. Therefore, these two elements
88 were included in the chemicals of concern list. Several other metals were present as impurities;
89 however, these metals were present at low levels (< 1 % of the MRSG product). According to
90 Golder Associates of Australia (reported in 2014), the metals which need to be monitored when
91 MRSG is land applied are arsenic (As), cadmium (Cd), selenium (Se), strontium (Sr) and zinc
92 (Zn).
93
94 The aims of this study were: 1) To determine the impact of MRSG application on the
95 environmental quality of the soils, plant tissue, oil and the surface water; and 2) To investigate
96 the uptake heavy metals by the oil palm and its oil quality.
97
98 2.0 Materials and Methods
99 2.1 Experimental site
Open
4
100 The study was conducted in an oil palm plantation in Bera, Pahang (GPS 03.27362 N, 102.58044
101 E). The soil in the plantation was formed on the rocks of Bera Formation of Permian age (Figure
102 1).
103
104 2.2 Investigating soil properties at the study site
105 A 3-year field trial was conducted, beginning in 2015, to test the efficacy of MRSG as a source
106 of Mg fertilizer at an oil palm plantation in Bera, Peninsular Malaysia. The results of the field
107 trial on the agronomic effects and soil/nutrient loss will be published elsewhere. A soil survey
108 was carried out to determine the soil series and subsequently classified them according to Soil
109 Taxonomy (Soil Survey Staff, 2014).
110
111 2.3 Experimental layout
112 The experimental design used was randomized complete block design (RCBD). There are five
113 treatments applied as shown in Table 1. These treatments are replicated in four blocks (Figure 2).
114 Each plot comprised six palms. Each treatment plot is separated by a small ditches and the
115 blocks are separated by larger drains to prevent trans-boundary movement of the applied
116 materials. Topsoil samples in each block of the field trial were collected to obtain the baseline
117 data (before treatment). The NPK fertilizers required to sustain oil palm growth/production were
118 applied every 6 months at the appropriate rates. MRSG, kieserite, and GML were applied 4 times
119 in the experimental plots were broadcasted and ploughed under to a depth of 15 cm within the
120 weeded circle of each palm (1.5 m from the trunk base) at an interval of six months. Only soil
121 from the highest MRSG application rate (T3) and the control (Chinese kieserite) (T4) treatments
122 were sampled and analysed.
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123 2.4 Sampling of soils
124 Topsoils from all experimental blocks were sampled and analyzed to get the baseline data before
125 applying the treatments (Figure 2). Soil samplings after MRSG application were carried out five
126 times as shown in Table 5. The soils were sampled in the weeded circle for each palm in the plot
127 and were composited.
128
129 2.5 Sampling of surface water
130 The surface water flowed from east to west (from point 1 to point 5) (Figure 2). Point 1 to point
131 3 is the stream receiving runoff water from the experimental plots. Point 4 and 5 represents the
132 water of the river before receival of water from the stream and after receiving water from the
133 stream, respectively, and can be used as a control. For the EMP, the samplings of the water were
134 carried out six times as shown in Table 6. The water were sampled a day after rainfall events.
135
136 For the purpose of comparing the EMP values of the surface water, data from all the three points of the
137 stream were pooled as a value for the stream, while the value for the river were taken from the average
138 value of the two points in the river. All water samples collected for laboratory analysis were kept
139 in an ice box of temperature below 4oC and added with several drops of HNO3 acid to control
140 pH below 2. These water samples were kept in a refrigerator below 4oC in the lab before
141 analysis. Water analysis followed the standard methods proposed by APHA (2005). The stream
142 values were compared with those of river using t-test as well as the water quality indices.
143
144 2.6 Sampling of oil palm tissue
145 Frond 17 is the indicator frond to show the nutrient status of matured palm. To get the baseline
146 data, frond 17 of the oil palm in the research plots were sampled for tissue analysis before
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147 treatments were applied. Frond 17 were chosen since it reflects single nutrient critical level in oil
148 palm. The oil palm tissues for the analyses after MRSG application were sampled four times as
149 shown in Table 8.
150 2.7 Sampling of fruitlets for the determination of palm oil quality
151 Oil palm fruitlets for extracting the oil to analyze heavy metals and other trace elements of
152 concern in it were sampled at the end of the project duration. This was about 2 years after MRSG
153 was first applied in the research plots. About 30 fruitlets were collected from each palm
154 harvested from each experimental plot and were put in separate envelopes. Overall, there were
155 180 fruitlets collected from each treatment in each block. In total, there were 720 fruitlets
156 collected and were brought to the laboratory. A quarter of these fruitlets were then randomly
157 chose and the mesocarp were chipped and composited for oil extraction.
158
159 2.8 Mineralogical Analysis of MRSG
160 The MRSG used in the current study was grounded to powder form and was mounted onto a
161 diamond stud to be examined under Field Emission Scanning Electron Microscope (FESEM).
162 The elements present were identified using the Energy Dispersive X-ray (EDX) attached to the
163 FESEM. The mineralogical composition (%) of the MRSG was determined by XRD analysis.
164
165 2.9 Chemical analyses of MRSG
166 Elemental composition of MRSG was extracted using the aqua-regia (3:1 ratio of concentrated
167 HCl to concentrated HNO3 acid) extractant and determined by ICP-OES. The elements
168 determined include La, As, Cd, Ce, Se, Sr and Zn.
169
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170 2.10 Determination of soil physico-chemical properties
171 Determination of the soil particle-size distribution (sand, silt, and clay) of the topsoil was carried
172 out by the pipette method developed by Olmstead et al., (1930). The clay fraction of the topsoil
173 was determined by Xray. Soil pH was determined at soil to water ratio of 1:2.5. Cation exchange
174 capacity (CEC) was determined by the summation method of McLean (1965). Basic
175 exchangeable cations were extracted using 100 mL of 1 M ammonium acetate buffered at pH 7.
176 The concentration of Ca and Mg in the solutions was determined by atomic absorption
177 spectrophotometer (AAS). Available P was extracted using Bray and Kurtz No. 2 extractant and
178 determined by the method of Murphy and Riley (1962), while organic C was determined by the
179 method of Walkley-Black (1947). Total carbon and total N in the soil were determined by dry
180 combustion techniques, using LECO CR-412 Carbon Analyser. Exchangeable Al was extracted
181 using 1 M KCl and Al in the extract was measured by inductively coupled plasma optical
182 emission spectrometry (ICP-OES).
183
184 2.11 Analysis of heavy metals and other elements of concern in soil
185 One gram of air-dried soil containing rare earth (Ce, La) and other elements of concern (As, Cd,
186 Se, Sr, Th, Zn, B, Mn, Pb, Cr, Ag, Ba, Al and Hg) was treated with nitric acid and perchloric
187 acid at the ratio of 3:1 with the addition of hydrogen peroxide (USEPA, 1996). The samples were
188 then digested on a hot plate. The metals and other elements of concern in the solution were
189 determined by ICP-MS Perkin Elmers Elan 9000 Model.
190
191
192
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193 2.12 Analysis of heavy metals and other elements of concern in surface water
194 The surface water collected from the stream and river were analyzed by the method of APHA
195 (2005) and determined using ICP-MS Perkin Elmers Elan 9000 Model.
196
197 2.13 Analysis of heavy metals and other elements of concern in oil palm tissue
198 Oil palm tissues from frond 17 were analyzed for the presence of heavy metals and other
199 elements of concern using wet digestion method. The elements were extracted with nitric acid
200 and hydrogen peroxide at the ratio of 3:1 as proposed by US EPA (1996). The elements
201 determined by ICP-MS were As, Cd, Ce, La, Se, Sr, Th, Zn, B, Mn, Pb, Cr, Ag, Ba, Al and Hg.
202
203 2.14 Extraction of palm oil from fruitlets and analysis of heavy metals and elements of
204 concern in the oil
205 Oil palm fruitlets sampled from fresh fruit bunches (FFB) were brought to the laboratory in
206 Universiti Putra Malaysia, Serdang to get its oil extracted. The mesocarp of the oil palm fruitlets
207 was chopped into small pieces and subsequently weighed before wrapping them with filter paper
208 inside a thimble. The wrapped mesocarp was later placed into a flask and hexane was added as
209 the solvent. The extraction of the oil was automatically run by a Soxhlet Unit (Gerhardt
210 Soxtherm). After 4 hours of extraction, the extracted oil was placed in an oven to let all the
211 remaining solvent to evaporate. When a constant weight of the oil was obtained, the oil
212 extraction rate (OER) was determined using the method of National Research Centre of Oil Palm
213 (2008).
214
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215 The oil extracted from oil palm fruitlets was analyzed by ICP-MS. The results obtained were
216 compared to those of the other edible oils as reported by Ashraf (2014), Zhu et al. (2011),
217 Pehlivan et al. (2008) and Mendil et al. (2009).
218
219 2.15 Determination of pollution indices
220 There are several ways to determine the pollution indices, which are:-
221 2.15.1 Biological Accumulation Coefficient
222 The Biological Accumulation Coefficient (BAC), which is an indicator of the ability of a plant to
223 accumulate a specific metal in contrast to the concentration of the metal in the soil substrate
224 (Ghosh and Singh, 2005) was calculated by equation 1 as follows:
225
226 (Equation1)---------------
227
228 where, heavy metal concentration in the edible parts of the plant and the soil are represented by
229 metal concentration in plant and metal concentration in soil, respectively.
230 2.15.2 Geo-accumulation Index
231
232 Established by Muller (1969), the Geo-accumulation Index (I-geo) was used to discover how
233 much metal has built up in soils/sediments and has been employed in a number of applications
234 and research purposes. I-geo is mathematically expressed in equation 2 below:
235 (Equation 2)------------- I-geo = log2 (Cn/1.5Bn)
236 where:
237 Cn = Concentration of element in the soil sample
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238 Bn = Geochemical background value.
239 Table A. Geochemical background value, Bn, based on shale
Bn value (in mg/kg)*
Co 19
Cr 90
Cu 45
Fe 47200
Mn 850
Ni 68
Zn 95
As 13
Cd 0.3
Ce 59
La 92
Se 0.6
Sr 300
Th 12
Pb 20
Ag 0.07
Ba 580
Hg 0.4
B 100
U 3.7
240 * Muller (1969)
241 A factor of 1.5 is used in the equation, in order to take into consideration the chance of
242 disparities in background data because of lithogenic factors. The geo-accumulation index (I-geo)
243 scale is made up of seven levels (0 – 6), from no contamination (0) to heavy pollution (6).
244 2.15.3 Pollution Load Index
245 The Pollution Load Index (PLI) is gathered as contamination Factors (CF), which is the quotient
246 given by dividing the metals concentration by a baseline concentration for each metal.
247 Concentration factor CF is made of four levels (0 – 3, low CF to high CF) (Hakanson, 1980).
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248 The PLI of the site was estimated by gathering the n-root from the CFs which were found from
249 the metals the PLI gathered from each location (Soares et al., 1999). The pollution load index
250 (PLI) was created by Tomlinson et al. (1980) as it is seen below:
251 CF = Cmetal / Cbackground value.
252 where:
253 CF = contamination factor,
254 n = number of metals
255 C metal = metal concentration in soil sample
256 C Background value = background value of that metal.
257 According to Cabrera et al. (1999), a PLI value equal to 1 signifies the absence of pollution,
258 while when PLI > 1 the soil is considered polluted.
259
260 2.16 Quality assurance
261
262 Quality assurance/quality control (QA/QC) was addressed by including blanks and replicates for
263 the water, soil, and plant tissue samples. Standard Reference Material (SRM) of National
264 Institute and Technology (NIST, 1640a for water), SRM-2711a Montana II Soil, and CRM-
265 LGC7162 Strawberry leaf) and internal reference materials were used for precision, quality
266 assurance and control (QA/QC) for selected metal measurements. Average values of three
267 replicates were taken for each determination. The precision of analytical procedures was
268 expressed as Relative Standard Deviation (RSD) which ranged from 5-15% and was calculated
269 from the standard deviation divided by the mean. The recovery rates of studied metals were
270 within 85±15%. Chemicals, stock solutions, and reagents were obtained from
271 Sigma/Fluka/Merck and were of analytical grade. All glassware were washed with distilled
272 water, soaked in nitric acid (30%) overnight, rinsed in deionized water and air-dried before use.
273
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274 2.17 Statistical analysis
275 All data on EMP were statistically analyzed by ANOVA for analysis of variance using Microsoft
276 Excel and significance between mean separations were tested using the t-test.
277
278 3.0 Results and discussion
279 3.1 Morphological and mineralogical characterization of the MRSG
280 The study area was occupied by the rocks of Bera Formation of Permian age (Shafeea et al.,
281 2000), which formed the soil of Jempol Series. The parent material is shale mixed with tuff
282 (Shafeea et al., 2000). Having high amount of clay content throughout its depth, the color of the
283 soil was reddish, indicating the presence of hematite, proven by XRD analysis. Morphological
284 observation of the soil profile in the soil pit showed the presence of an argillic diagnostic horizon
285 (Bt). The occurrence of the Bt horizon was confirmed by the significant accumulation of the clay
286 content in that zone. The presence of other iron minerals, goethite and hematite, resulted in the
287 phenomenon of low CEC; this notion was consistent with the findings of Shamshuddin et al.
288 (1991) and Ismail et al. (1993).
289
290 The soil was moderately well-drained, which was suitable for oil palm production (Shamshuddin
291 et al., 2018). The somewhat slow water movement down the soil profile was due in part to the
292 presence of more than 75% clay in the soil. Organic matter content in topsoil was high, mostly
293 contributed partly by the debris from the cut fronds and/or empty fruit bunches, which had been
294 laid out in the inter-row of the oil palm. Due to the presence of Bt horizon together with low
295 exchangeable Ca and Mg as well as low CEC, the soil was classified as an Ultisol as defined by
296 the Soil Survey Staff (2014).
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297 The topsoil pH was 4.4, meaning that Al was present in a soluble form which, to a certain extent,
298 affected oil palm growth (Table 3). At this pH level, Al3+ in the soil solution would be
299 hydrolysed, resulting in further decrease of soil pH. Oil palm may be able to grow normally on
300 the soil as it is acid-tolerant, which can even survive at the soil pH of 4.3 (Auxtero and
301 Shamshuddin, 1991). In the topsoil, the exchangeable Ca (0.64 cmolc/kg) and Mg (0.23
302 cmolc/kg) were within the normal limit for an Ultisol of the tropics. The main problem with soil
303 for oil palm production is the lack of Mg and/or Ca.
304 Figure 3 shows the FESEM micrograph of the MRSG under study. The acicular-shaped mineral
305 in the micrograph was gypsum. The elements present at the three locations (spectrum 1, 2 and 3)
306 in the micrograph were identified by FESEM-EDX (Figure 4). A spectrum analysis indicating
307 the presence of certain elements were made.
308
309 3.2 Chemical characterization of the MRSG
310 The level of their concentration was below the critical limit set by the Standard and Industrial
311 Research Institute of Malaysia (SIRIM) and the Department of Agriculture (DOA) (Table 2),
312 which are the relevant authorities/agencies in Malaysia responsible for introducing guidelines for
313 the usage of schedule wastes on agriculture land. The concentration of As and Cd in the MRSG
314 were far below the guideline limit. It means that the MRSG used in the current study has the
315 potential to be safely applied on agricultural land for oil palm production.
316
317 3.3 Physico-chemical properties of the soil in the study area
318 The soil was sampled prior to treatments application and also during the duration of the
319 experiment.
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320 3.3.1 The baseline data on soil
321 The topsoil in the experimental blocks before the application of MRSG was analysed and the
322 results are presented in Table 3 (for physico-chemical properties) and Table 4 (for heavy metals
323 and other elements of concern). These data were used as baseline information that could be used
324 for comparison after applying MRSG.
325
326 Soil data presented in Table 3 indicated that the soil was fertile having moderately high
327 exchangeable Ca, Mg and K, which were rather uncommon for an Ultisol cropped to oil palm in
328 Peninsular Malaysia. The soil samples from the 4 experimental blocks analysed for the baseline
329 data were taken from the weeded circle as well as in the inter-rows of the oil palm in the
330 plantation where cut fronds and/or empty fruit bunches were once laid down as mulching
331 materials to conserve water or to keep the soil moist. This notion was evidence by the presence
332 of high amount of organic matter (Table 3). On the other hand, the concentration of heavy metals
333 and other elements of concern in the soil from the experimental blocks (Table 4) were below the
334 guidelines set by SIRIM and DOA presented in Table 2.
335
336 3.4 Effects of MRSG application on soil
337 Determination of the soil quality (Table 5) was based on various indices, namely Biological
338 Accumulation Coefficient (BAC) (Ghosh and Singh, 2005), Geological Index (I-geo) (Muller,
339 1969), Contamination Factor (CF) Hakanson (1980) and Pollution Load Index (PLi) (Tomlinson
340 et al., 1980). Heavy metals content and other elements of concern present in the soil under study
341 (Table 5) and those of the surface water (Table 6) were evaluated based on the above-mentioned
342 indices and the results are presented in Table 7. The results showed that the BAC was low to
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343 moderate for As, Cd and Se, and was intensive for Zn. However, intensive level for Zn was
344 probably not due to the result of applying MRSG as small amount of Zn was present in the
345 MRSG (Table 2). Note that Zn is a micronutrient; hence, it is needed in small amount to sustain
346 the growth of the oil palm in the plantation and/or for its FFB production.
347
348 The level of heavy metals present in the treated soil was lower than their respective value or
349 reference (Table 5). The heavy metals contents and other elements of concern in the soil of the
350 experimental plots were below the soil investigation level, which means the concentrations of a
351 contaminant above which further appropriate investigation and evaluation will be required
352 (Zarcinas et al., 2004) and Eco-SSL (USEPA, 2007). Heavy metals and other elements of
353 concern in the surface water before and after MRSG application were below the bench mark
354 value of Ministry of Health Malaysia (2000) (Table 6). The drinking water standard of Malaysia
355 is adopted from World Health Organizations standard. Environmental risk analysis (Table 7)
356 showed that the soil was not contaminated, evidenced by the low contamination factor
357 (Hakanson, 1980) with low pollution load index (Tomlinson et al., 1980).
358
359 The content of the heavy metals and other elements of concern in the soil of the research plots in
360 the study area were not affected by the application of MRSG, kieserite and GML, with no
361 significant differences among treatments (Table 5). This means that MRSG and kieserite
362 treatment had produced comparable or similar results.
363
364 The critical toxic concentration of La and Ce in soils throughout the world is unavailable at the
365 moment. However, the mean concentration of the two rare earth elements in some common soils
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366 of Japan and China had been determined; the respective concentration was 18 and 40 mg/kg,
367 while that of Chinese soils was 44 and 86 mg/kg. For the topsoil in the forest of Sweden, the
368 corresponding concentration was 5-5-33.2 and 11-68 mg/kg (Tyler, 2004). It is believed that their
369 concentration in the soil under study due to MRSG application would not exceed the amount
370 present in the soils of Japan or China, which were evidenced from data presented in Table 5. For
371 Sr, according to Forum of European Geological Survey (FOREGS, 2018) database, its median
372 concentration in the topsoil is 89.0 mg/kg and 0.50 mg/L in water.
373
374 3.5 Effect of MRSG application on surface water quality
375 Heavy metals and other elements of concern in the surface water before and after MRSG
376 application were below the bench mark value of Ministry of Health Malaysia (2000) for all the
377 sampling dates (Table 6). There are no significant differences between the concentration of
378 TEOC between the stream and the river in the study site. The pH of surface water was slightly
379 acidic. The values were fluctuating slightly through the study period. The pH of water in the
380 surface water were within the Class IV of the NWQS standard.
381
382 3.6 Effects of MRSG application on oil palm tissue
383 During the course of its growth, the oil palm in the plantation under production had taken up all
384 sorts of plant nutrients as well as other elements contained in the soil on which it was growing
385 that could be detected in the leaves. The concentration of the heavy metals in the oil palm tissue
386 from frond 17 was not affected by treatments (Table 8). Hence; there was no significant
387 difference in the results due to treatment with MRSG and kieserite.
388
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389 Cytotoxic (As, Cd, and Se) and phytotoxic (Zn) elements have also been determined in the oil
390 palm tissues (Table 8). Based on the results of the EMP carried out during the period of the 3-
391 year field trial, it was concluded that application of MRSG as Mg fertilizer source in the oil palm
392 plantation was not significantly different from the baseline data. Therefore, long-term application
393 of MRSG in the plantation can be beneficial for oil palm growth and its yield in terms of fresh
394 fruit bunches as it was able to supply the much needed Mg, Ca and S, required to sustain its
395 growth and/or production.
396
397 3.7 Effects of MRSG application on palm oil
398 The ultimate test on the impact of applying MRSG on the soil cropped to oil palm is the quality
399 of its oil which was still within the acceptable levels in terms of the heavy metals content and the
400 elements of concern. The concentration of the said elements in the palm oil presented in Table 9
401 was compared to those of the edible oils on sale at the marketplace shown in Table 10. The
402 results of the comparison did not show any indication of the accumulation of heavy metals and
403 other elements of concern in the palm oil under investigation. This is in line with the finding of
404 other studies by Violina et al. (2011); Sengalevitch (1999); Szyczewski et al. (2016) and Tyler
405 (2004) on oil crops that show there is little accumulation of heavy metals in the oil. This study
406 shows that in the extracted oil, the heavy metals were much lower than those found/reported by
407 other researchers (Table 10). Palm oil quality resulting from the soil being treated with MRSG
408 and kieserite were similar.
409 To further enhance the conclusion of this study, cytotoxic (As, Cd, and Se) and phytotoxic (Zn)
410 elements have also been determined in the palm oil (Table 9). The results showed that both
411 groups of elements were below the known guideline limit.
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412 4.0 Conclusion
413 The results of the field trial in Bera, Peninsular Malaysia showed that MRSG application could
414 bring about positive impact on Malaysian palm oil industry. The quality of the palm oil was not
415 significantly affected by the application of MRSG, producing results similar with those of the
416 kieserite. It was also proven that MRSG application did not result in negative impact on the
417 environment; thus, the quality of the soil and surface water in the oil palm plantation and/or in
418 the surrounding area remained intact. The respective phytotoxic and cytotoxic elements in the
419 tissues of the oil palm and palm oil were below the concentration of other studies. Furthermore,
420 long-term application of MRSG in the oil palm plantation could have positive impact on the
421 fresh fruit bunches production. Hence, it is recommended that MRSG be applied in oil palm
422 plantations in Peninsular Malaysia occupied by the highly weathered Ultisols to sustain palm oil
423 production in the long run.
424
425 Acknowledgements
426 The authors would like to thank Lynas Malaysia Sdn Bhd for the financial support. We also want
427 to express our gratitude to Universiti Putra Malaysia as well as Universiti Kebangsaan Malaysia
428 for the technical support. The approval by the Department of Environment, Malaysia for
429 allowing us to use the MRSG for research purposes is highly appreciated. We also wish to thank
430 individuals or group of people, either in or outside the country, who in one way or another helped
431 towards the successful and timely implementation of the research project in good time.
432
433
434
435
436
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536 in the region of KCM-AD-Plovdiv. Prilozenieza ekologia kam bjuletin KCM 1999, 1, 10-17.
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538 Shafeea, M.L., Kamal, R. M., Sone, M., 2000. On the new Permian Bera Formation from Bera
539 District, Pahang, Malaysia. Proc. Ann. Geol. Conf., Penang. 151-158.
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541 Shamshuddin, J., Che Fauziah, I., Sharifuddin, H.A.H., 1991. Effects of limestone and gypsum
542 applications to a Malaysian Ultisol on soil solution composition and yields of maize and groundnut.
543 Plant Soil. 134, 45-52. doi: 10.1007/BF00010716.
544
545 Shamshuddin, J., Ismail, H., 1995. Reactions of ground magnesium limestone and gypsum in
546 soils with variable-charge minerals. Soil Sci. Soc. America J. 59(1), 106-112.
547
548 Shamshuddin, J., Fauziah, C.I., 2010. Weathered Tropical Soils: the Ultisols and Oxisols. UPM
549 Press, Serdang, Malaysia.
550
551 Shamshuddin, J., Fauziah, C.I., Roslan, I., Noordin, W. D., 2018. Ultisols and Oxisols:
552 Enhancing their Productivity for Oil Palm, Rubber and Cocoa Cultivation. 2nd edition. UPM
554
555 Soares, H. M., Boaventura, R. A. R., Esteves da Silva, J., 1999. Sediments as monitors of heavy
556 metal contamination in the Ave river basin (Portugal): multivariate analysis of data. Environ.
557 Poll. 105, 311-323. doi: 10.1016/S0269-7491(99)00048-2.
558
559 Soil Survey Staff, 2014. Keys to Soil Taxonomy. United States Department of Agriculture, 12 th
560 Edition, Washington DC.
561
562 Szyczewski, P., Marcin, F., Anetta, Z., Jerzy, S., Tomasz, S., Paweł, P., 2016. A comparative
563 study of the content of heavy metals in oils: linseed oil, rapeseed oil and soybean oil in
564 technological production processes. Archives of Environ. Protect. 42(3),37–40. Doi:
565 10.1515/aep-2016-0029.
566
567 The New Dutch List, 2000. Target values, Soil Remediation Intervention Values and Indicative
568 Levels for Serious Contamination. Department of Soil Protection, The Hague, Netherland.
569
570 Tomlinson, D.L., Wilson, J.G., Harris, C.R., Jeffney, D.W., 1980. Problems in the assessment of
571 heavy metal levels in estuaries and the formation of a pollution index. Helgol. Wiss.
572 Meeresunters. 33, 566-572. doi: 10.1007/BF02414780.
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573
574 Tyler, G., 2004. Rare earth elements in soil and plant system - A review. Plant and Soil. 267,
575 191-206. doi: 10.1007/s11104-005-4888-2.
576
577 US EPA, 1996. Method 3050B: Acid Digestion of Sediments, Sludges, and Soils, in: Selected
578 Analytical Methods for Environmental Remediation and Recovery (SAM).
579 https://www.epa.gov/homeland-security-research/epa-method-3050b-acid-digestion-sediments-
580 sludges-and-soils. (Accessed on February 5, 2018).
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582 US EPA, 2007. Guidance for Developing Ecological Soil Screening Levels.
583 https://www.epa.gov/sites/production/files/201509/documents/ecossl_guidance_chapters.pdf.
584 (Accessed February 5, 2018).
585
586 Violina, A., Radka, I., Ivanov, K., 2005. Heavy metal accumulation and distribution in oil crops.
587 Commun. in Soil Sci. Plant Anal. 35(17-18), 2551-2566, doi: 10.1081/LCSS-200030368.
588
589 Walkley, A., 1947. A critical examination of a rapid method for determination of organic carbon
590 in soils - effect of variations in digestion conditions and of inorganic soil constituents. Soil Sci.
591 63, 51-257.
592
593 Zarcinas, B.A., Ishak, C.F., McLaughlin, M.J., Cozens, G., 2004. Heavy metals in soils and
594 crops in Southeast Asia. 1. Peninsular Malaysia. Environ. Geochem. Health. 26(4), 343-357.
595 doi:10.1007/s10653-005-4669-0.
596
597 Zhu, F., Fan, W., Wang, X., Qu, L., Yao, S., 2011. Health risk assessment of eight heavy metals
598 in nine varieties of edible vegetable oils consumed in China. Food Chem. Toxic. 49(12), 3081-
599 3085. doi:10.1016/j.fct.2011.09.019.
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*Graphical Abstract
YIELD
FACTORY
OIL
Heavy Metal:
As, Cd, Cu, Fe, Mn,
By-product Pb, Zn
(MRSG) FROND 17
Trace Elements of
Concern (TEOC):
0 – 25 cm
Se, Ce, La, Sr, Th, B
Weeded circle
SURFACE WATER
SOIL
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*Highlights (for review : 3 to 5 bullet points (maximum 85 characters including spaces per bullet point)
 MRSG supplies Mg and Ca for oil palm growth

 Metal content in soil, plant tissue and oil are below the permitted concentration
 Oil palm treated with MRSG produces non-cytotoxic oil, hence is safe for
consumption
 MRSG application does not affect the soil, plant tissue, water and palm oil quality
 MRSG is practical and sustainable as a soil amendment in oil palm plantation
*Revised manuscript with no changes marked (double-spaced and continuously LINE and PAGE numbered)
Click here to view linked References
1 Impact of Mg Rich Synthetic Gypsum Application on the Environment and Palm Oil
2 Quality
3
4 Sahibin1, A. R., J. Shamshuddin2, C.I. Fauziah2*, O. Radziah2, I. Wan Mohd Razi3 and M.S.K.
5 Enio4
6
1
7 Environmental Science Program, Faculty of Science and Natural Resources, Universiti Malaysia
8 Sabah, 88400 Kota Kinabalu, Sabah, Malaysia
9
2
10 Department of Land Management, Faculty of Agriculture, Universiti Putra Malaysia, 43400
12
3
13 School of Environmental and Natural Resources Sciences, Faculty of Science and Technology,
14 Universiti Kebangsaan Malaysia, 43600 Bangi, Selangor, Malaysia
15
4
16 Department of Science and Technical Education, Faculty of Educational Studies, Universiti
17 Putra Malaysia, 43400 Serdang, Selangor, Malaysia
18
*
19 Correspondence: cfauziah@upm.edu.my; Tel: +603-8947 4938
20
21 Abstract
22 A study was conducted in an oil palm plantation in Peninsular Malaysia to elucidate the effects
23 of applying Magnesium Rich Synthetic Gypsum (MRSG), a by-product of chemical plant, on the
24 chemical properties of soil, the uptake of heavy metals by the palm trees, the oil quality and its
25 impact on the surrounding environment. The results showed that MRSG application onto soil
26 cropped to oil palm could bring positive impact in terms of soil chemical properties and oil palm
27 production. The quality of the oil was not significantly affected by the continuous MRSG
28 application as shown by the low heavy metals and trace elements of concern content (Cu: 0.062
29 mg/kg; Fe: 2.10 mg/kg; Mn: 1.93 mg/kg; Pb: 0.006 mg/kg; Zn: 0.103 mg/kg; Cr: 0.354 mg/kg;
30 Ni: 0.037 mg/kg). From the I-geochem index, the soil was found to have values ranging from -
31 3.81 to -1.03 which is considered as uncontaminated. Further, its application did not result in
32 negative impact on the surrounding environment; hence, the quality of the soil and surface water
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33 in the plantation and/or the surrounding area remained intact. Phytotoxic elements in the oil palm
34 tissue (As: 0.12 mg/kg; Se: 0.05 mg/kg; Zn: 1.48 mg/kg; Ce: 0.47 mg/kg; La: 0.26 mg/kg; Sr:
35 3.03 mg/kg) and cytotoxic elements in the oil were below the acceptable limit. Based on the
36 results of the Environmental Monitoring out during the period of the study, it was concluded that
37 application of the by-product of the chemical plant as a source of Mg to enhance soil fertility in
38 the oil palm plantation was considered safe and sustainable. The effects of applying MRSG and
39 Chinese kieserite was almost similar. So, MRSG can be used as a possible source of Mg to
40 replace Chinese kieserite for oil palm production on the Ultisols in Peninsular Malaysia.
41 Keywords: cytotoxic; heavy metals; kieserite; magnesium; rare earth element
42
43 1.0 Introduction
44 Over the last few decades, the main sources of magnesium fertilizer for oil palm plantation in
45 Malaysia are kieserite from Germany and ground magnesium limestone (GML) which is locally
46 mined. Synthetic magnesium sulphate from China (Chinese kieserite) has also made some in
47 road since the late 1990’s although its scale of use is significantly less than the two fertilizers
48 stated earlier.
49
50 The high price of Germany kieserite and low reactivity of GML make it feasible for the
51 plantation industry to seek for an alternative source of magnesium fertilizer. The chemical plant
52 in Malaysia that extract rare earth elements produces a by-product called Neutralization
53 Underflow (NUF) residue. This material, also called Mg Rich Synthetic Gypsum (MRSG), can
54 be applied in oil palm plantations as a source of Mg fertilizer. The MRSG is classified as
55 Scheduled Waste (SW205) by the Department of Environment (DoE), Ministry of Natural
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56 Resources and Environment, Malaysia (DOE, 1974). The Atomic Energy Licensing Board
57 (AELB, 2008) of Malaysia had confirmed that MRSG was non-radioactive. It means that the
58 material has the potential to be utilized in agriculture. It is therefore worthwhile to determine if
59 this MRSG can replace the imported kieserite as Mg source to sustain oil palm growth and palm
60 oil production in the long run. Since this by-product contains some trace elements of concern
61 (TEOC) (As, Cd, Se, Zn, Ce, La and Sr), so its impact on the environment needs to be evaluated
62 before it can be recommended for application. However, there were several studies that showed
63 very little accumulation of heavy metals in upper plant biomass of oil crops as reported by
64 Violina et al. (2005); Sengalevitch (1999); Szyczewski et al. (2016) and Tyler (2004).
65
66 Malaysia has currently more than 5 million ha cultivated with oil palm, which constitutes the
67 biggest arable land area allocated to agriculture in the country. Soils in Peninsular Malaysia used
68 for growing oil palm are Ultisols, dominated by kaolinite, gibbsite, goethite and hematite in the
69 clay fraction (Shamshuddin and Ismail, 1995; Shamshuddin and Fauziah, 2010). According to
70 Shamshuddin et al. (1991), the cation exchange capacity (CEC) of Ultisols was low, resulting in
71 low retention in the soil and thus low availability of Mg and Ca that limits crop productivity.
72 With low pH, Al3+ is present in amount that affects the growth oil palm roots.
73
74 Oil palm productivity is limited by the infertile nature of the soils; hence, fertilizer application
75 become an important issue to sustain production. Ultisols usually have plant nutrients
76 insufficient for normal production, unless they are adequately fertilized. About 60% of the cost
77 of palm oil production comes from fertilizer that requires to supply the needed nutrients.
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78 Ca, Mg and S are needed by oil palm under production in high amount for its healthy growth
79 and/or production, and it is believed that these macronutrients can be added into soils in the
80 plantations by continuous application of MRSG. Besides, by virtue of being alkaline (the pH of
81 MRSG is 8.8), due to the presence of magnesium hydroxide, calcium hydroxide and some
82 calcium carbonate, soil pH can be raised to the desired level for oil palm cultivation.
83 Furthermore, MRSG contained some Si that may help prevent certain oil palm disease prevailing
84 in the plantations throughout the country (Najihah et al., 2014).
85
86 Components of MRSG include rare earth compounds lanthanum (La) and cerium (Ce); both
87 were present at about 1 %. However, La and Ce are cytotoxic. Therefore, these two elements
88 were included in the chemicals of concern list. Several other metals were present as impurities;
89 however, these metals were present at low levels (< 1 % of the MRSG product). According to
90 Golder Associates of Australia (reported in 2014), the metals which need to be monitored when
91 MRSG is land applied are arsenic (As), cadmium (Cd), selenium (Se), strontium (Sr) and zinc
92 (Zn).
93
94 The aims of this study were: 1) To determine the impact of MRSG application on the
95 environmental quality of the soils, plant tissue, oil and the surface water; and 2) To investigate
96 the uptake heavy metals by the oil palm and its oil quality.
97
98
99
100
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101
102 2.0 Materials and Methods
103 2.1 Experimental site
104 The study was conducted in an oil palm plantation in Bera, Pahang (GPS 03.27362 N, 102.58044
105 E). The soil in the plantation was formed on the rocks of Bera Formation of Permian age (Figure
106 1).
107
108 2.2 Investigating soil properties at the study site
109 A 3-year field trial was conducted, beginning in 2015, to test the efficacy of MRSG as a source
110 of Mg fertilizer at an oil palm plantation in Bera, Peninsular Malaysia. The results of the field
111 trial on the agronomic effects and soil/nutrient loss will be published elsewhere. A soil survey
112 was carried out to determine the soil series and subsequently classified them according to Soil
113 Taxonomy (Soil Survey Staff, 2014).
114
115 2.3 Experimental layout
116 The experimental design used was randomized complete block design (RCBD). There are five
117 treatments applied as shown in Table 1. These treatments are replicated in four blocks (Figure 2).
118 Each plot comprised six palms. Each treatment plot is separated by a small ditches and the
119 blocks are separated by larger drains to prevent trans-boundary movement of the applied
120 materials. Topsoil samples in each block of the field trial were collected to obtain the baseline
121 data (before treatment). The NPK fertilizers required to sustain oil palm growth/production were
122 applied every 6 months at the appropriate rates. MRSG, kieserite, and GML were applied 4 times
123 in the experimental plots were broadcasted and ploughed under to a depth of 15 cm within the
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124 weeded circle of each palm (1.5 m from the trunk base) at an interval of six months. Only soil
125 from the highest MRSG application rate (T3) and the control (Chinese kieserite) (T4) treatments
126 were sampled and analysed.
127
128 2.4 Sampling of soils
129 Topsoils from all experimental blocks were sampled and analyzed to get the baseline data before
130 applying the treatments (Figure 2). Soil samplings after MRSG application were carried out five
131 times as shown in Table 5. The soils were sampled in the weeded circle for each palm in the plot
132 and were composited.
133
134 2.5 Sampling of surface water
135 The surface water flowed from east to west (from point 1 to point 5) (Figure 2). Point 1 to point
136 3 is the stream receiving runoff water from the experimental plots. Point 4 and 5 represents the
137 water of the river before receival of water from the stream and after receiving water from the
138 stream, respectively, and can be used as a control. For the EMP, the samplings of the water were
139 carried out six times as shown in Table 6. The water were sampled a day after rainfall events.
140
141 For the purpose of comparing the EMP values of the surface water, data from all the three points of the
142 stream were pooled as a value for the stream, while the value for the river were taken from the average
143 value of the two points in the river. All water samples collected for laboratory analysis were kept
144 in an ice box of temperature below 4oC and added with several drops of HNO3 acid to control
145 pH below 2. These water samples were kept in a refrigerator below 4oC in the lab before
146 analysis. Water analysis followed the standard methods proposed by APHA (2005). The stream
147 values were compared with those of river using t-test as well as the water quality indices.
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148
149 2.6 Sampling of oil palm tissue
150 Frond 17 is the indicator frond to show the nutrient status of matured palm. To get the baseline
151 data, frond 17 of the oil palm in the research plots were sampled for tissue analysis before
152 treatments were applied. Frond 17 were chosen since it reflects single nutrient critical level in oil
153 palm. The oil palm tissues for the analyses after MRSG application were sampled four times as
154 shown in Table 8.
155
156 2.7 Sampling of fruitlets for the determination of palm oil quality
157 Oil palm fruitlets for extracting the oil to analyze heavy metals and other trace elements of
158 concern in it were sampled at the end of the project duration. This was about 2 years after MRSG
159 was first applied in the research plots. About 30 fruitlets were collected from each palm
160 harvested from each experimental plot and were put in separate envelopes. Overall, there were
161 180 fruitlets collected from each treatment in each block. In total, there were 720 fruitlets
162 collected and were brought to the laboratory. A quarter of these fruitlets were then randomly
163 chose and the mesocarp were chipped and composited for oil extraction.
164
165 2.8 Mineralogical Analysis of MRSG
166 The MRSG used in the current study was grounded to powder form and was mounted onto a
167 diamond stud to be examined under Field Emission Scanning Electron Microscope (FESEM).
168 The elements present were identified using the Energy Dispersive X-ray (EDX) attached to the
169 FESEM. The mineralogical composition (%) of the MRSG was determined by XRD analysis.
170
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171
172 2.9 Chemical analyses of MRSG
173 Elemental composition of MRSG was extracted using the aqua-regia (3:1 ratio of concentrated
174 HCl to concentrated HNO3 acid) extractant and determined by ICP-OES. The elements
175 determined include La, As, Cd, Ce, Se, Sr and Zn.
176
177 2.10 Determination of soil physico-chemical properties
178 Determination of the soil particle-size distribution (sand, silt, and clay) of the topsoil was carried
179 out by the pipette method developed by Olmstead et al., (1930). The clay fraction of the topsoil
180 was determined by Xray. Soil pH was determined at soil to water ratio of 1:2.5. Cation exchange
181 capacity (CEC) was determined by the summation method of McLean (1965). Basic
182 exchangeable cations were extracted using 100 mL of 1 M ammonium acetate buffered at pH 7.
183 The concentration of Ca and Mg in the solutions was determined by atomic absorption
184 spectrophotometer (AAS). Available P was extracted using Bray and Kurtz No. 2 extractant and
185 determined by the method of Murphy and Riley (1962), while organic C was determined by the
186 method of Walkley-Black (1947). Total carbon and total N in the soil were determined by dry
187 combustion techniques, using LECO CR-412 Carbon Analyser. Exchangeable Al was extracted
188 using 1 M KCl and Al in the extract was measured by inductively coupled plasma optical
189 emission spectrometry (ICP-OES).
190
191 2.11 Analysis of heavy metals and other elements of concern in soil
192 One gram of air-dried soil containing rare earth (Ce, La) and other elements of concern (As, Cd,
193 Se, Sr, Th, Zn, B, Mn, Pb, Cr, Ag, Ba, Al and Hg) was treated with nitric acid and perchloric
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194 acid at the ratio of 3:1 with the addition of hydrogen peroxide (USEPA, 1996). The samples were
195 then digested on a hot plate. The metals and other elements of concern in the solution were
196 determined by ICP-MS Perkin Elmers Elan 9000 Model.
197
198 2.12 Analysis of heavy metals and other elements of concern in surface water
199 The surface water collected from the stream and river were analyzed by the method of APHA
200 (2005) and determined using ICP-MS Perkin Elmers Elan 9000 Model.
201
202 2.13 Analysis of heavy metals and other elements of concern in oil palm tissue
203 Oil palm tissues from frond 17 were analyzed for the presence of heavy metals and other
204 elements of concern using wet digestion method. The elements were extracted with nitric acid
205 and hydrogen peroxide at the ratio of 3:1 as proposed by US EPA (1996). The elements
206 determined by ICP-MS were As, Cd, Ce, La, Se, Sr, Th, Zn, B, Mn, Pb, Cr, Ag, Ba, Al and Hg.
207
208 2.14 Extraction of palm oil from fruitlets and analysis of heavy metals and elements of
209 concern in the oil
210 Oil palm fruitlets sampled from fresh fruit bunches (FFB) were brought to the laboratory in
211 Universiti Putra Malaysia, Serdang to get its oil extracted. The mesocarp of the oil palm fruitlets
212 was chopped into small pieces and subsequently weighed before wrapping them with filter paper
213 inside a thimble. The wrapped mesocarp was later placed into a flask and hexane was added as
214 the solvent. The extraction of the oil was automatically run by a Soxhlet Unit (Gerhardt
215 Soxtherm). After 4 hours of extraction, the extracted oil was placed in an oven to let all the
216 remaining solvent to evaporate. When a constant weight of the oil was obtained, the oil
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217 extraction rate (OER) was determined using the method of National Research Centre of Oil Palm
218 (2008).
219 The oil extracted from oil palm fruitlets was analyzed by ICP-MS. The results obtained were
220 compared to those of the other edible oils as reported by Ashraf (2014), Zhu et al. (2011),
221 Pehlivan et al. (2008) and Mendil et al. (2009).
222
223 2.15 Determination of pollution indices
224 There are several ways to determine the pollution indices, which are:-
225 2.15.1 Biological Accumulation Coefficient
226 The Biological Accumulation Coefficient (BAC), which is an indicator of the ability of a plant to
227 accumulate a specific metal in contrast to the concentration of the metal in the soil substrate
228 (Ghosh and Singh, 2005) was calculated by equation 1 as follows:
229
230 (Equation1)---------------
231
232 where, heavy metal concentration in the edible parts of the plant and the soil are represented by
233 metal concentration in plant and metal concentration in soil, respectively.
234 2.15.2 Geo-accumulation Index
235
236 Established by Muller (1969), the Geo-accumulation Index (I-geo) was used to discover how
237 much metal has built up in soils/sediments and has been employed in a number of applications
238 and research purposes. I-geo is mathematically expressed in equation 2 below:
239 (Equation 2)------------- I-geo = log2 (Cn/1.5Bn)
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240 where:
241 Cn = Concentration of element in the soil sample
242 Bn = Geochemical background value.
243 Table A. Geochemical background value, Bn, based on shale
Bn value (in mg/kg)*
Co 19
Cr 90
Cu 45
Fe 47200
Mn 850
Ni 68
Zn 95
As 13
Cd 0.3
Ce 59
La 92
Se 0.6
Sr 300
Th 12
Pb 20
Ag 0.07
Ba 580
Hg 0.4
B 100
U 3.7
244 * Muller (1969)
245 A factor of 1.5 is used in the equation, in order to take into consideration the chance of
246 disparities in background data because of lithogenic factors. The geo-accumulation index (I-geo)
247 scale is made up of seven levels (0 – 6), from no contamination (0) to heavy pollution (6).
248
249 2.15.3 Pollution Load Index
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250 The Pollution Load Index (PLI) is gathered as contamination Factors (CF), which is the quotient
251 given by dividing the metals concentration by a baseline concentration for each metal.
252 Concentration factor CF is made of four levels (0 – 3, low CF to high CF) (Hakanson, 1980).
253 The PLI of the site was estimated by gathering the n-root from the CFs which were found from
254 the metals the PLI gathered from each location (Soares et al., 1999). The pollution load index
255 (PLI) was created by Tomlinson et al. (1980) as it is seen below:
256 CF = Cmetal / Cbackground value.
257 where:
258 CF = contamination factor,
259 n = number of metals
260 C metal = metal concentration in soil sample
261 C Background value = background value of that metal.
262 According to Cabrera et al. (1999), a PLI value equal to 1 signifies the absence of pollution,
263 while when PLI > 1 the soil is considered polluted.
264
265 2.16 Quality assurance
266
267 Quality assurance/quality control (QA/QC) was addressed by including blanks and replicates for
268 the water, soil, and plant tissue samples. Standard Reference Material (SRM) of National
269 Institute and Technology (NIST, 1640a for water), SRM-2711a Montana II Soil, and CRM-
270 LGC7162 Strawberry leaf) and internal reference materials were used for precision, quality
271 assurance and control (QA/QC) for selected metal measurements. Average values of three
272 replicates were taken for each determination. The precision of analytical procedures was
273 expressed as Relative Standard Deviation (RSD) which ranged from 5-15% and was calculated
274 from the standard deviation divided by the mean. The recovery rates of studied metals were
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275 within 85±15%. Chemicals, stock solutions, and reagents were obtained from
276 Sigma/Fluka/Merck and were of analytical grade. All glassware were washed with distilled
277 water, soaked in nitric acid (30%) overnight, rinsed in deionized water and air-dried before use.
278
279 2.17 Statistical analysis
280 All data on EMP were statistically analyzed by ANOVA for analysis of variance using Microsoft
281 Excel and significance between mean separations were tested using the t-test.
282
283 3.0 Results and discussion
284 3.1 Morphological and mineralogical characterization of the MRSG
285 The study area was occupied by the rocks of Bera Formation of Permian age (Shafeea et al.,
286 2000), which formed the soil of Jempol Series. The parent material is shale mixed with tuff
287 (Shafeea et al., 2000). Having high amount of clay content throughout its depth, the color of the
288 soil was reddish, indicating the presence of hematite, proven by XRD analysis. Morphological
289 observation of the soil profile in the soil pit showed the presence of an argillic diagnostic horizon
290 (Bt). The occurrence of the Bt horizon was confirmed by the significant accumulation of the clay
291 content in that zone. The presence of other iron minerals, goethite and hematite, resulted in the
292 phenomenon of low CEC; this notion was consistent with the findings of Shamshuddin et al.
293 (1991) and Ismail et al. (1993).
294
295 The soil was moderately well-drained, which was suitable for oil palm production (Shamshuddin
296 et al., 2018). The somewhat slow water movement down the soil profile was due in part to the
297 presence of more than 75% clay in the soil. Organic matter content in topsoil was high, mostly
298 contributed partly by the debris from the cut fronds and/or empty fruit bunches, which had been
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299 laid out in the inter-row of the oil palm. Due to the presence of Bt horizon together with low
300 exchangeable Ca and Mg as well as low CEC, the soil was classified as an Ultisol as defined by
301 the Soil Survey Staff (2014).
302
303 The topsoil pH was 4.4, meaning that Al was present in a soluble form which, to a certain extent,
304 affected oil palm growth (Table 3). At this pH level, Al3+ in the soil solution would be
305 hydrolysed, resulting in further decrease of soil pH. Oil palm may be able to grow normally on
306 the soil as it is acid-tolerant, which can even survive at the soil pH of 4.3 (Auxtero and
307 Shamshuddin, 1991). In the topsoil, the exchangeable Ca (0.64 cmolc/kg) and Mg (0.23
308 cmolc/kg) were within the normal limit for an Ultisol of the tropics. The main problem with soil
309 for oil palm production is the lack of Mg and/or Ca.
310
311 Figure 3 shows the FESEM micrograph of the MRSG under study. The acicular-shaped mineral
312 in the micrograph was gypsum. The elements present at the three locations (spectrum 1, 2 and 3)
313 in the micrograph were identified by FESEM-EDX (Figure 4). A spectrum analysis indicating
314 the presence of certain elements were made.
315
316 3.2 Chemical characterization of the MRSG
317 The level of their concentration was below the critical limit set by the Standard and Industrial
318 Research Institute of Malaysia (SIRIM) and the Department of Agriculture (DOA) (Table 2),
319 which are the relevant authorities/agencies in Malaysia responsible for introducing guidelines for
320 the usage of schedule wastes on agriculture land. The concentration of As and Cd in the MRSG
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321 were far below the guideline limit. It means that the MRSG used in the current study has the
322 potential to be safely applied on agricultural land for oil palm production.
323 3.3 Physico-chemical properties of the soil in the study area
324 The soil was sampled prior to treatments application and also during the duration of the
325 experiment.
326
327 3.3.1 The baseline data on soil
328 The topsoil in the experimental blocks before the application of MRSG was analysed and the
329 results are presented in Table 3 (for physico-chemical properties) and Table 4 (for heavy metals
330 and other elements of concern). These data were used as baseline information that could be used
331 for comparison after applying MRSG.
332
333 Soil data presented in Table 3 indicated that the soil was fertile having moderately high
334 exchangeable Ca, Mg and K, which were rather uncommon for an Ultisol cropped to oil palm in
335 Peninsular Malaysia. The soil samples from the 4 experimental blocks analysed for the baseline
336 data were taken from the weeded circle as well as in the inter-rows of the oil palm in the
337 plantation where cut fronds and/or empty fruit bunches were once laid down as mulching
338 materials to conserve water or to keep the soil moist. This notion was evidence by the presence
339 of high amount of organic matter (Table 3). On the other hand, the concentration of heavy metals
340 and other elements of concern in the soil from the experimental blocks (Table 4) were below the
341 guidelines set by SIRIM and DOA presented in Table 2.
342
343 3.4 Effects of MRSG application on soil
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344 Determination of the soil quality (Table 5) was based on various indices, namely Biological
345 Accumulation Coefficient (BAC) (Ghosh and Singh, 2005), Geological Index (I-geo) (Muller,
346 1969), Contamination Factor (CF) Hakanson (1980) and Pollution Load Index (PLi) (Tomlinson
347 et al., 1980). Heavy metals content and other elements of concern present in the soil under study
348 (Table 5) and those of the surface water (Table 6) were evaluated based on the above-mentioned
349 indices and the results are presented in Table 7. The results showed that the BAC was low to
350 moderate for As, Cd and Se, and was intensive for Zn. However, intensive level for Zn was
351 probably not due to the result of applying MRSG as small amount of Zn was present in the
352 MRSG (Table 2). Note that Zn is a micronutrient; hence, it is needed in small amount to sustain
353 the growth of the oil palm in the plantation and/or for its FFB production.
354
355 The level of heavy metals present in the treated soil was lower than their respective value or
356 reference (Table 5). The heavy metals contents and other elements of concern in the soil of the
357 experimental plots were below the soil investigation level, which means the concentrations of a
358 contaminant above which further appropriate investigation and evaluation will be required
359 (Zarcinas et al., 2004) and Eco-SSL (USEPA, 2007). Heavy metals and other elements of
360 concern in the surface water before and after MRSG application were below the bench mark
361 value of Ministry of Health Malaysia (2000) (Table 6). The drinking water standard of Malaysia
362 is adopted from World Health Organizations standard. Environmental risk analysis (Table 7)
363 showed that the soil was not contaminated, evidenced by the low contamination factor
364 (Hakanson, 1980) with low pollution load index (Tomlinson et al., 1980).
365
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366 The content of the heavy metals and other elements of concern in the soil of the research plots in
367 the study area were not affected by the application of MRSG, kieserite and GML, with no
368 significant differences among treatments (Table 5). This means that MRSG and kieserite
369 treatment had produced comparable or similar results.
370
371 The critical toxic concentration of La and Ce in soils throughout the world is unavailable at the
372 moment. However, the mean concentration of the two rare earth elements in some common soils
373 of Japan and China had been determined; the respective concentration was 18 and 40 mg/kg,
374 while that of Chinese soils was 44 and 86 mg/kg. For the topsoil in the forest of Sweden, the
375 corresponding concentration was 5-5-33.2 and 11-68 mg/kg (Tyler, 2004). It is believed that their
376 concentration in the soil under study due to MRSG application would not exceed the amount
377 present in the soils of Japan or China, which were evidenced from data presented in Table 5. For
378 Sr, according to Forum of European Geological Survey (FOREGS, 2018) database, its median
379 concentration in the topsoil is 89.0 mg/kg and 0.50 mg/L in water.
380
381 3.5 Effect of MRSG application on surface water quality
382 Heavy metals and other elements of concern in the surface water before and after MRSG
383 application were below the bench mark value of Ministry of Health Malaysia (2000) for all the
384 sampling dates (Table 6). There are no significant differences between the concentration of
385 TEOC between the stream and the river in the study site. The pH of surface water was slightly
386 acidic. The values were fluctuating slightly through the study period. The pH of water in the
387 surface water were within the Class IV of the NWQS standard.
388
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389
390
391 3.6 Effects of MRSG application on oil palm tissue
392 During the course of its growth, the oil palm in the plantation under production had taken up all
393 sorts of plant nutrients as well as other elements contained in the soil on which it was growing
394 that could be detected in the leaves. The concentration of the heavy metals in the oil palm tissue
395 from frond 17 was not affected by treatments (Table 8). Hence; there was no significant
396 difference in the results due to treatment with MRSG and kieserite.
397
398 Cytotoxic (As, Cd, and Se) and phytotoxic (Zn) elements have also been determined in the oil
399 palm tissues (Table 8). Based on the results of the EMP carried out during the period of the 3-
400 year field trial, it was concluded that application of MRSG as Mg fertilizer source in the oil palm
401 plantation was not significantly different from the baseline data. Therefore, long-term application
402 of MRSG in the plantation can be beneficial for oil palm growth and its yield in terms of fresh
403 fruit bunches as it was able to supply the much needed Mg, Ca and S, required to sustain its
404 growth and/or production.
405
406 3.7 Effects of MRSG application on palm oil
407 The ultimate test on the impact of applying MRSG on the soil cropped to oil palm is the quality
408 of its oil which was still within the acceptable levels in terms of the heavy metals content and the
409 elements of concern. The concentration of the said elements in the palm oil presented in Table 9
410 was compared to those of the edible oils on sale at the marketplace shown in Table 10. The
411 results of the comparison did not show any indication of the accumulation of heavy metals and
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412 other elements of concern in the palm oil under investigation. This is in line with the finding of
413 other studies by Violina et al. (2011); Sengalevitch (1999); Szyczewski et al. (2016) and Tyler
414 (2004) on oil crops that show there is little accumulation of heavy metals in the oil. This study
415 shows that in the extracted oil, the heavy metals were much lower than those found/reported by
416 other researchers (Table 10). Palm oil quality resulting from the soil being treated with MRSG
417 and kieserite were similar.
418
419 To further enhance the conclusion of this study, cytotoxic (As, Cd, and Se) and phytotoxic (Zn)
420 elements have also been determined in the palm oil (Table 9). The results showed that both
421 groups of elements were below the known guideline limit.
422
423 4.0 Conclusion
424 The results of the field trial in Bera, Peninsular Malaysia showed that MRSG application could
425 bring about positive impact on Malaysian palm oil industry. The quality of the palm oil was not
426 significantly affected by the application of MRSG, producing results similar with those of the
427 kieserite. It was also proven that MRSG application did not result in negative impact on the
428 environment; thus, the quality of the soil and surface water in the oil palm plantation and/or in
429 the surrounding area remained intact. The respective phytotoxic and cytotoxic elements in the
430 tissues of the oil palm and palm oil were below the concentration of other studies. Furthermore,
431 long-term application of MRSG in the oil palm plantation could have positive impact on the
432 fresh fruit bunches production. Hence, it is recommended that MRSG be applied in oil palm
433 plantations in Peninsular Malaysia occupied by the highly weathered Ultisols to sustain palm oil
434 production in the long run.
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435
436
437 Acknowledgements
438 The authors would like to thank Lynas Malaysia Sdn Bhd for the financial support. We also want
439 to express our gratitude to Universiti Putra Malaysia as well as Universiti Kebangsaan Malaysia
440 for the technical support. The approval by the Department of Environment, Malaysia for
441 allowing us to use the MRSG for research purposes is highly appreciated. We also wish to thank
442 individuals or group of people, either in or outside the country, who in one way or another helped
443 towards the successful and timely implementation of the research project in good time.
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Table
Click here to download Table: Table 5Oct.docx
Table 1. GML, MRSG and kieserite applied in the research plots
Treatment Rate of application
T0 (Control 1) 1.25 kg/palm application of GML
T1 1.1 kg/palm application of MRSG
T2 1.45 kg/palm application of MRSG
T3* 2.4 kg/palm application of MRSG
T4 (Control 2)* 0.5 kg/palm application of kieserite
*Only these treatment plots were sampled for TEOC

Table 2. Heavy metals and other elements of concern in MRSG and the guidelines limit by
SIRIM and DOA
SIRIM DOA
Golder
MRSG Associates Guidelines
Material Guidelines
(this study) Report limit Guidelines
Limit
(2014) Regulation limit +
MS1517:2012,
7(1) MS1517:2012 φ
MS2532:2013
Gypsum (%) 54.6 75-95
Mg hydroxide (%) 5-12
Calcium <1
Oxides/hydroxide (%)
Calcium carbonate (%) 1-3
Silica (amorphous) (%) 0.1-0.4
Silicon (%) bdl
Lanthanum hydroxide <1
(%)
Lanthanum (%) 0.33
Cerium hydroxide (%) <1
Arsenic (mg/kg) bdl 500 50 50
Cadmium (mg/kg) 0.80 N.A. 5 5
Cerium (mg/kg) 3460.53 N.A N.A N.A
Lanthanum (mg/kg) 3272.49 N.A N.A N.A
Selenium (mg/kg) 0.35 3500 N.A N.A
Strontium (mg/kg) 85.21 N.A N.A N.A
Zinc (mg/kg) 38.63 N.A. N.A N.A
bdl= below detection limit
+
MS1517:2012: Organic Fertilizers-Specification (1st Revision); N.A = not available
φ
MS2532:2013: Fortified Organic Fertilizers-Specification
Table 3. The baseline data of the studied area for the EMP
Soil parameter Block

1 2 3 4 S.D
Sand (%) 11.00 9.00 7.00 5.00 2.39
Very Coarse sand 2-1 mm 1.16 1.12 0.50 0.22 0.43
Coarse sand 1.0-0.5mm 1.46 1.40 1.42 0.72 0.33
Medium sand 0.5-0.25mm 2.28 1.89 1.32 1.15 0.48
Fine sand 0.25-0.125 mm 2.98 2.20 1.96 1.52 0.57
Very fine sand 0.125-0.063mm 3.12 2.39 1.80 1.39 0.70
silt (%) 0.063-0.002mm 14.00 17.00 17.00 10.00 3.07
Clay (%) <0.002mm 75.00 74.00 76.00 86.00 5.15
Organic matter (%) 6.63 8.72 7.34 7.27 0.81
Organic carbon (%) 1.74 2.10 1.86 1.77 0.15
pH Water (1:2.5) 4.33 4.54 4.44 4.40 0.08
Electrical Conductivity (µS/cm) 2480 2460 2390 2410 38.91
Exchangeable Al (cmolc/kg) 0.90 0.05 0.06 0.10 0.38
Exchangeable H (cmolc/kg) 0.70 0.40 0.40 0.40 0.14
Exchangeable Ca (cmolc/kg) 0.97 1.20 1.24 0.87 0.17
Exchangeable Mg (cmolc/kg) 0.98 1.12 0.80 0.71 0.17
Exchangeable Na (cmolc/kg) 0.06 0.05 0.04 0.05 0.01
Exchangeable K (cmolc/kg) 0.61 0.26 0.24 0.50 0.17
Cation exch capacity (cmolc/kg) 4.22 3.04 2.73 3.04 0.61
Total N (%) 2.36 2.30 2.14 2.30 0.09
Total S (%) 0.16 0.11 0.15 0.10 0.03
Total C (%) 2.17 3.28 2.79 2.54
0.43
*S.D= standard deviation
Table 4. Heavy metals and other elements of concern in the soil of the oil palm plantation
before treatment
Block
1 2 3 4
Element mg/kg
As 1.44 0.60 0.17 0.12

Cd 0.01 0.01 0.01 0.01
Ce 2.31 4.96 1.61 2.96
La 0.91 2.26 1.21 1.00
Se 1.09 2.00 1.61 2.07
Sr 2.31 1.93 2.12 1.50
Th 0.83 0.13 0.98 0.87
Zn 14.56 16.60 15.86 13.93
B 1.50 0.66 1.75 0.85
Mn 144.97 709.61 187.86 174.36
Table 5. Heavy metals and other elements of concern in the soil before and after MRGS application
# @
Metal 12/3/15 05/10/2015 22/1/2016 22/5/2016 20/9/2016 *Soil CSQ Eco-SSL
(mg/kg) Baseline Investigati G (mg/kg)
on Levels (mg/k
(mg/kg) g)
Cont MRSG Cont MRSG Cont MRSG Cont MRSG
As 1.75 4.50 5.07 1.40 1.93 1.67 0.82 2.57 1.50 60 12 18
cd b b d cd d e c d
Cd 0.03 bdl bdl 0.002 0.03 0.04 0.02 0.03 0.03 0.3 1.4 32
b c b b b b b
Se 0.65 0.83 0.77 0.08 0.06 0.60 0.73 0.43 0.58 NA 1.0 0.52
ab a a d d b a c b
Zn 19.82 15.31 17.40 12.36 15.08 5.82 5.39 2.09 1.94 95 200 160
a b a c b d d e e
Ce 6.16 4.18 5.78 10.70 13.97 2.87 2.32 4.77 3.89 NA NA NA
c c c b a d d c c
La 2.64 1.63 2.38 7.15 7.11 1.15 1.09 1.91 1.83 NA NA NA
c d c a a e e cd cd
Sr 5.07 2.57 5.30 1.79 2.25 2.15 0.46 11.58 20.04 NA NA NA
c d c d d d e b a
Means followed by different letter within same row are significantly different at p≤0.05
bdl= below detection limit; NA=not available; Cont = control
*Zarcinas et al. (2004); #CSQG= Canadian Soil Quality Guidelines (CCME, 2007)
@ Ecological Soil Screening Level for plant as a receptor (USEPA, 2007)
Table 6. Heavy metals and other elements of concern in the surface water before and after MRSG application
*Benchm
Metal
22/5/2016 20/9/2016 29/11/2016 10/5/2017 ark
(µg/L)
(µg/L)
Stream River Stream River Stream River Stream River
As 0.85 1.01 1.03 1.69 1.75 3.74 1.79 1.84 10
a a b a b a a a
Cd 0.02 0.03 0.23 0.09 0.05 0.08 0.06 0.06 3
a a a b a a a a
Se 0.22 0.28 0.06 0.19 0.24 0.30 0.06 0.14 10
a a b a a a b a
Zn 105.20 135.39 51.02 63.67 61.51 35.10 56.27 49.39 3000
a a a a a b a a
Ce 0.41 0.82 1.29 1.31 0.60 0.60 3.11 2.33 NA
a a a a a a a b
La 0.16 0.37 0.55 0.62 0.24 0.30 1.25 1.00 NA
a a a a a a a a
Sr 18.30 22.58 9.46 26.88 12.66 25.96 18.54 30.79 NA
a a b a b a b a
pH 5.08a 5.02a 5.73b 5.97a 6.00a 6.02a 5.78a 5.08b 5-9#
Means followed by different letter from each rainfall event are significantly different at p≤0.05 for each element
*Ministry of Health Malaysia (2000); NA= not available
#Malaysian Environmental Quality Report (2006) (Class IV).
Table 7. Biological Accumulation Coefficient of heavy metals in frond 17 and soil contamination levels following MRSG treatment
Metal Index* Value Note

As BAC 0.31 Moderate
I-geo -2.97 Uncontaminated
CF 0.29 low CF
Cd BAC 0.90 Moderate
CF 0.14 low CF
Se BAC 0.34 Moderate
CF 0.90 low CF
Zn BAC 1.16 Intensive
CF 0.14 low CF
PLi 0.70 Not polluted
*
BAC - Biological Accumulation Coefficient; Igeo - Geological Index;
CF- Contamination Factor; and PLI - Pollution Load Index
Table 8. Heavy metals and other elements of concern in frond 17
*Normal or
Metal 5/10/2015
22/1/2016 22/5/2016 21/7/2016 1/12/2016 Sufficient
(mg/kg) Baseline
(mg/kg)
Control MRSG Control MRSG Control MRSG Control MRSG Control MRSG
1.38 0.88 0.41 0.50 2.32 2.30 0.64 0.70 0.11 0.12
As 1-1.7
b c e e a a d d f f
0.02 0.02 0.005 0.08 0.03 0.03 0.29 0.29 0.04
Cd bdl 0.05-0.2
d d e b cd cd a a c
0.18 0.04 0.12 0.17 0.08 0.09 0.54 0.44 0.04 0.05
Se 0.01-2
c e d c d d a b e e
42.73 46.70 31.51 22.55 20.01 17.09 20.48 23.05 4.26 1.48
Zn 27-150
a a b c c d c c e f
0.36 0.22 2.32 4.12 2.31 1.95 0.55 0.55 0.43 0.47
Ce NA
d e b a b b c c cd d
0.28 0.22 1.69 3.81 1.42 1.24 0.61 0.55 0.21 0.26
La NA
e f b a bc c d d f e
10.61 8.84 6.37 7.26 5.03 4.71 16.76 18.89 2.11 3.03
Sr NA
b c cd c d d a a e e
*Kabata-Pendias (2011); NA= not available; bdl=below detection limit
Table 9. Heavy metals and other elements of concern in the palm oil
T0 T1 T2 T3 T4
Element
(ppm)
0.0690 0.0600 0.0580 0.0430 0.1220
Al
a a a a ab
bdl bdl bdl bdl bdl
As
a a a a a
bdl bdl 0.0001 bdl bdl
Cd
ab b a b ab
0.0001 0.0014 0.0024 0.0016 0.0028
Ce
b ab ab ab ab
0.0004 0.0007 0.0014 0.0001 0.0013
La
b ab a ab ab
bdl bdl bdl bdl bdl
Se
a a a a a
0.0240 0.0160 0.0130 0.0160 0.0100
Sr
a a a a a
bdl bdl bdl bdl bdl
Th
a a a a a
0.1030 0.0700 0.0430 0.0420 0.0520
Zn
a a a a a
0.0210 0.0200 0.0170 1.9300 0.0190
Mn
a a a a a
0.0040 0.0060 0.0050 0.0020 0.0040
Pb
a a a a a
0.0090 0.0060 0.0080 0.3540 0.0090
Cr
a a a a a
0.0001 0.0001 bdl bdl bdl
Ag
ab a c c bc
0.0100 0.0090 0.0120 0.0130 0.0070
Ba
a a a a a
bdl bdl bdl bdl bdl
B
a a a a a
bdl bdl bdl bdl bdl
Hg
a a a a a
0.0100 0.0050 0.0040 0.0370 0.0030
Ni
a a a a a
0.0560 0.0620 0.0300 0.0260 0.0250
Cu
a a a a a
0.0010 0.0030 0.0030 0.0090 0.0030
Co
a a a a a
0.0010 0.0010 0.0020 0.0020 0.0030
Mo
a a a a a
1.1530 0.6300 0.6200 0.6290 1.0400
Si
a a a a a
0.2280 0.7050 0.1050 2.0990 0.2240
Fe
a a a a a
bdl=below detection limit
Table 10. Concentration of heavy metals in edible oils
Metal
(mg/kg) Corn Sunflower Soybean Peanut Sesame Olive Rapeseed Palm Reference
Oil oil oil oil oil oil oil
As 0.011 0.013 0.016 0.017 0.018 0.013 0.018 - (1)
0.012 0.011 0.015 0.013 0.019 0.012 0.015 - (2)
0.002 (5)
- (6)
- (7)
bdl this study
Cd 0.006 0.003 0.005 0.004 0.006 0.002 0.006 - (1)
0.008 0.004 0.004 0.004 0.005 0.003 0.006 - (2)
0.045 (5)
0.065 (6)
- (7)
bdl this study
Cu 0.035 0.062 0.052 0.178 0.049 0.286 0.193 - (1)
0.0138 0.0026 0.073 - - 0.0155 - - (3)
1.200 (6)
0.4 (7)
0.062 this study
Fe 17.3 33.4 24.3 37.8 43.8 57.8 26.8 - (1)
52 105.3 - - - 139 - - (4)
0.0195 0.0107 0.0129 - - 0.0295 - - (3)
130 (6)
5.0 (7)
2.10 this study
Mn 0.097 0.347 0.13 0.586 0.269 0.186 0.178 - (1)
1.64 0.12 - - - 0.14 - - (4)
0.0017 0.0026 0.022 - - 0.0065 - - (3)
9.250 (6)
- (7)
1.930 this study
Pb bdl 0.011 0.014 0.013 0.017 bdl 0.011 - (1)
0.009 0.01 0.015 0.012 0.018 0.013 0.012 - (2)
bdl 0.0016 bdl - - 0.0074 - - (3)
0.038 (5)
0.042 (6)
- (7)
0.006 this study
Zn 3.1 1.54 1.36 1.78 0.955 1.88 1.67 - (1)
2.56 1.23 0.742 1.3 0.883 1.41 1.57 - (2)
3.08 1.10 - - - 1.03 - - (4)
8.470 (6)
- (7)
0.103 this study
1) Ashraf (2014), (2) Zhu et al. (2011), (3) Pehlivan et al. (2008), (4) Mendil et al. (2009), (5)
Adepoju-bello et al. (2012), (6) Nnorom et al. (2014), (7) FAO/WHO (2015); bdl=below detection
limit
Figure
Click here to download Figure: Figures 5Oct.docx
Figure 1. The geology map of Bera area, Pahang, Peninsular Malaysia

(modified from Mohd Shafeea et al., 2000)
(A=Bera Formation; B= Semantan Formation; C= Sandstone)
*2 columns image
Figure 2. Diagrammatic representation of the experimental blocks in the study area; the red
diamonds indicated the sites where surface water was sampled
*2 columns image
Figure 3. FESEM micrograph of the MRSG used in the study
*Single column image

Figure 4. FESEM-EDX diffractogram of the MRSG
*Single column image

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Elsevier Editorial System(tm) for Science of

the Total Environment

Manuscript Number: STOTEN-D-18-07582R1

Title: Impact of Mg Rich Synthetic Gypsum Application on the Environment

Article Type: Research Paper

Keywords: cytotoxic; heavy metals; kieserite; magnesium; rare earth

Corresponding Author: Dr. Che Fauziah Ishak, Ph.D.

Corresponding Author's Institution:

First Author: Sahibin Abd Rahim, PhD

Abstract: A study was conducted in an oil palm plantation in Peninsular

Response to Reviewers: Abstract: To rewrite again, please avoid to repeat

Line 53: delete "The" at the beginning of the sentence

Line 54:…..presence "of "Al3+

Lines 56-59: repetitive, please rephrase

Line 68. Add the reference/year

Line 73: to rephrase! It's the same as line 72

Line 75: replace "quantity" by "amount"

Line79: to rephrase! It's the same as line 75

Lines 83-84: not clear. If the concentration of rare elements compounds

Response to Reviewer comment: The reason is La and Ce are cytotoxic

In my opinion is better to start with the description of the study area

Lines 111-114: what was the criteria to choose the "appropriate

Lines 129-130: repetitive…..-baseline data- and -reference information-

Response to Reviewer comment: Repetation has been removed.

Line 133: why from frond 17? Explain it.

Lines 133-134: what "appropriate times and locations" means? Is very

Lines 138-140: not clear, please explain it better

Lines 161-165: again, there is no details about the sampling itself.

Response to Reviewer comment: Has been improved accordingly.

Line 174: define "OER"

Line 215: " a factor of"

Lines 218-223: not clear, rephrase.

Lines 253-256: not clear and repetitive "the elements present….were

Lines 257-261: repetitive first you write "…detailed elemental

Line 261: define SIRIM and DOA.

Lines 263-264: in my opinion, Cd concentration is not that low. The

Section 3.2: instead of describing soil colors it would be better to

Lines 309-310: the whole sentence doesn't make sense.

Lines 334-336: define what a "soil investigation level" is.

Lines 348-356: more references about rare elements has to be included.

Line 377: is Th a harmful element?

Lines 387-392: this sentence looks more like a final conclusion.

Line 401: "palm oil safe limit" compared to what? Literature or

"Highly appreciated?" Personally I would use constructions like: the

Table 9: concentrations for As are 0? How is that possible? Response

Figure 1: for me this figure is pointless.

Figure 2: include GPS points within the map

Figure 3: typing error, block 2 (next to block 3) should be block 4.

Line 377: is Th a harmful element? Yes. It is slightly radioactive. But

41 Keywords: cytotoxic; heavy metals; kieserite; magnesium; rare earth element

54 be applied in oil palm plantations as a source of Mg fertilizer. The MRSG is classified as

55 Scheduled Waste (SW205) by the Department of Environment (DoE), Ministry of Natural

58 material has the potential to be utilized in agriculture. It is therefore worthwhile to determine if

80 plantations by continuous application of MRSG. Besides, by virtue of being alkaline (the pH of

84 in the plantations throughout the country (Najihah et al., 2014).

98 2.0 Materials and Methods

99 2.1 Experimental site

104 2.2 Investigating soil properties at the study site

109 Taxonomy (Soil Survey Staff, 2014).

111 2.3 Experimental layout

122 were sampled and analysed.

127 and were composited.