Journal of Cleaner Production 347 (2022) 131202

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Journal of Cleaner Production

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Adsorption-desorption kinetics and phosphorus loss standard curve in

erosive weathered granite soil: Stirred flow chamber experiments
Tianyu Sun a, b, Kai Fei a, b, Longzhou Deng a, b, Liping Zhang a, b, *, Xiaojuan Fan a, b,
Yanhong Wu a, b
a
Institute of Soil and Water and Environmental Sciences, College of Environment and Resource Sciences, Zhejiang University, Hangzhou, 310058, PR China
b
Zhejiang Provincial Key Laboratory of Agricultural Resources and Environment, Hangzhou, 310058, PR China

A R T I C L E I N F O A B S T R A C T

Handling Editor: Bin Chen Weathered granite has a high soil adsorption rate and it is difficult to apply phosphate fertilizers. In order to
effectively use phosphorus, it is very important to study the intensity and speed of soil retention and desorption
Keywords: of phosphorus. The purpose of this study is to evaluate the kinetics of adsorption and desorption in soils with
Phosphorus adsorption different erodibility. We selected three weathered granite soils with hugely different erosions: topsoil layer (TL-
Phosphorus desorption
Tillage layer), laterite layer (LL-Laterite layer) and sand layer (SL-Sand layer). Phosphorus adsorption and
Kinetics
desorption experiments were successively carried out in the stirred flow reaction chamber, and the stirred flow
Stirred flow method
Weathered granite experiment under unsaturated adsorption conditions was carried out for the first time. The maximum absorption
capacity (qamax) and desorption capacity (qdmax) of phosphorus in TL soil was both greater than that in LL and SL
soil. The adsorption process mainly occurs within the first 250 min of the reaction. The desorption ratio (Dr) in
the TL soil is smaller than the LL and SL soil. The order of the fast reaction sites proportion (F) is SL > LL > TL in
adsorption process and LL > SL > TL in desorption process. Seven key soil property indicators can fit qamax and
qdmax values well. In the determination coefficient (R2) of the standard curve of phosphorus loss, SL soil is the
larger than TL and LL. The qamax and Dr values measured in the stirred flow experiment are both larger than those
in the batch experiment. Among the three soils, LL has the lowest adsorption capacity for P and the highest
accessibility. The slow adsorption sites in TL account for the main part, and the adsorption in LL and SL mainly
occurs at fast adsorption sites. Through the establishment of the phosphorus loss standard curve, the maximum
phosphorus loss in the entire region can be predicted and calculated. This study can provide theoretical basis and
reference for phosphorus management in similar soil types or physical geographical areas with severely eroded
soils.

1. Introduction
In order to pursue a sustained and high yield of food, phosphorus has
become an indispensable additive for modern agriculture (Lun et al.,
2018). Phosphate fertilizer will increase short-term phosphorus export
potential soon after application, and increase long-term phosphorus
export potential by improving soil fertility. In China, crop yields have
increased significantly with the increase of phosphorus input, but the
utilization efficiency of phosphorus has been significantly reduced.
From 2004 to 2014, as the amount of phosphate fertilizer increased from
88 to 123 kg P2O5 ha− 1 yr− 1, the total phosphorus utilization efficiency
dropped from 68% to 20%, resulting in an accumulation of> 90 kg P2O5
ha− 1 yr− 1 year in the soil (Zhang et al., 2019). The application of
phosphorus for more than 350 years has obviously contributed a lot to
mankind (Smith et al., 2019), but the loss of phosphorus caused by
excessive application of phosphate fertilizer and runoff erosion (espe­
cially under heavy rain conditions) has also caused serious water
pollution (King et al., 2015; Ockenden et al., 2016; Osmond et al., 2019).
For example, the water quality degradation caused by accelerated algae
propagation, and the negative impact on fishery and other uses (Ho
et al., 2019; Le Moal et al., 2019). Phosphorus loss in agriculture has
become one of the key contributing factors to the eutrophication of
water bodies in China. In order to control and reduce phosphorus loss,
the study of phosphorus adsorption-desorption law and reaction

* Corresponding author. Institute of Soil and Water and Environmental Sciences, College of Environment and Resource Sciences, Zhejiang University, Hangzhou,
310058, PR China.
E-mail address: lpzhang@zju.edu.cn (L. Zhang).

https://doi.org/10.1016/j.jclepro.2022.131202
Received 1 July 2021; Received in revised form 7 February 2022; Accepted 1 March 2022
Available online 9 March 2022
0959-6526/© 2022 Elsevier Ltd. All rights reserved.
T. Sun et al. Journal of Cleaner Production 347 (2022) 131202

mechanism under runoff conditions is particularly critical. and iron ions on the adsorption and desorption of phosphorus in the soil
The adsorption and desorption laws of phosphorus in soil are often in a stirred flow experiment; (4) innovatively putting forward a pre­
studied by batch experiments to determine phosphorus adsorption iso­ diction method of soil phosphorus loss through the stirring flow
therms (Queiroz et al., 2021). The phosphorus adsorption value and experiment.
desorption capacity are mainly affected by the clay content, amorphous
aluminum and other physical and chemical indicators of soil (Gerard, 2. Materials and methods
2016; Soinne et al., 2014; Yang et al., 2019). Many current studies have
obtained key factors affecting soil adsorption and desorption charac­ 2.1. Study area
teristics in specific areas. In some studies, calculation models for the
maximum phosphorus adsorption and desorption ratio have been The experimental soil was taken from the weathered granite hillside
established (Sun et al., 2020). However, due to uneven fertilizer appli­ in Anji County, northwestern Zhejiang Province (N30◦ 35′ 18.59′′ ,
cation and differences in temporal and spatial accumulation, there is a E119◦ 18′ 54.76′′ , Fig. 1), which is a mid-subtropical monsoon region
large uncertainty in the fixed amount and loss of phosphorus in the field characterized by abundant rainfall and a mild climate. The soil type in
soil in a certain area. Therefore, it is difficult to make effective quanti­ this area is acid red soil developed with weathered granite as the matrix.
tative predictions of soil phosphorus adsorption value and runoff The base material has low phosphorus content and high iron oxide and
phosphorus loss, especially the quantitative model of phosphorus loss alumina content (Deng et al., 2019). Heavy rains and sloping fields
from underground runoff (soil flow) has not been seen (Djodjic and caused by frequent typhoons are very common in this area. Due to the
Markensten, 2019; Drohan et al., 2019). removal of topsoil and reduction of soil thickness caused by severe wind
Stirring flow method is a new type of phosphorus adsorption- and hydraulic damage, the area is exposed to different underlying soil
desorption law research method. Compared with traditional batch pro­ levels. Its erosion characteristics and development levels are usually
cessing technology, the reaction environment of this method is closer to representative of the erosive weathered granite area in southern China
the field conditions with low soil-water ratio, and it has the advantages (Liu, 2018; Wang et al., 2016).
of short equilibrium time and not affected by the concentration balance The sampling points are located on some typical slopes and are less
and diffusion process (Aharoni and Sparks, 1991). In the reaction affected by human intervention. Past studies have shown that the soil
chamber of the stirring flow experiment, the continuously inputted developed by weathered granite soil can be divided into cultivated layer,
adsorbent solution and the soil sample are continuously stirred, thus laterite layer, sand layer and clastic layer (Fig. 2) (Deng et al., 2020; Fei
maintaining the consistency of the adsorbent concentration in the re­ et al., 2019). The uppermost layer is the farming layer, which is then
action chamber and accelerating the formation of the eroded by wind and runoff, exposing the laterite layer. When severely
adsorption-desorption equilibrium state. This experimental design eroded, the sand layer will also be exposed. Therefore, we sampled three
greatly shortens the reaction time and avoids the potential impact on the differently eroded slope soils.
experimental results due to diffusion in the soil matrix (Bar-Tal et al.,
1990). This method was first used to improve the adsorption-desorption
kinetics of soil potassium ions (Carski and Sparks, 1985). Since the
1990s, the agitated flow experiment has been carried out on soil phos­
phorus adsorption-desorption kinetics one after another, mainly as a
supplement to batch experiments, to study the differences in soil phos­
phorus adsorption characteristics, loss rates and impact mechanisms
(Beauchemin et al., 1996; Guedes et al., 2016). For example, Fink et al.
(2016) studied the phosphorus adsorption-desorption kinetic parame­
ters of four highly weathered soils and their different mechanisms using
agitated flow method, and observed that most phosphorus adsorption
occurred in the first 100 min. Abdala et al. (2015) compared the dif­
ference in phosphorus desorption kinetics of highly weathered agricul­
tural soils with different fertilization years using the stirring flow
method, and evaluated the phosphorus cycle of fertilizers in the soil. Due
to the accuracy of the results and the wide applicability of the experi­
mental stirred flow, this technology has been used in soil analysis to
evaluate the adsorption and desorption kinetics of various elements such
as copper and zinc and organic matter (Alvarez-Esmoris et al., 2020;
Fernandez-Calvino et al., 2015a; Fernandez-Calvino et al., 2015b; Per­
ez-Novo et al., 2011a,b). However, at present, the stirring flow tech­
nology is rarely used to study and evaluate the kinetics of phosphorus in
the soil, and the quantitative prediction model of soil phosphorus
adsorption-desorption has not yet been seen. Therefore, this study hopes
to conduct a more accurate quantitative study and mechanism analysis
on the kinetics and adsorption-desorption behavior of phosphorus in the
soil through a stirred flow experiment, in order to provide suggestions
for the improvement of phosphorus fertilizer use efficiency and reduce
the loss caused by phosphorus loss Potential environmental pollution
risk.
The goals of this research are:(1) comparing the kinetic character­
istics of phosphate adsorption-desorption at different levels in erosive
weathered granite soil; (2) obtaining the main indicators affecting the
maximum soil phosphorus adsorption-desorption in the study area, and
establish a simulation calculation model of qamax and qdmax; (3) for the
first time, explaining the influence mechanism of the loss of aluminum Fig. 1. Location map of weathered granite soil sampling points.

2
T. Sun et al.
Fig. 2. Hierarchical view of the weathering crust from erosive granite.
2.2. Soil collection and analysis
Soil samples were collected from three different exposed soil layers.
The research is on soils with a depth of 60 cm for each soil layer. Four
soil mixture samples were collected at 15 cm intervals for each soil layer.
All of the mixed soil samples consist of three parallel samples in adjacent
areas. A total of 12 mixed samples were collected. The soil sample is air-
dried under natural conditions and sieved through a 2 mm screen.
X-ray fluorescence analysis method (XRF) was used to determine the
elemental composition of soil samples (XRF, ALL-9800, Thermo Fisher
Scientific, USA). The soil samples were pretreated by the mixed flux
fusion method (Haukka and Thomas, 1977). The amorphous Fe (Fea)and
Al(Ala) were extracted by 0.1 mol/L of oxalic acid solution and 0.2
mol/L ammonium oxalate at pH 3 (de Campos et al., 2016). Iron and
aluminum content in the extracts were measured with inductively
coupled plasma optical emission spectroscopy (ICP-OES, ICP6000,
Thermo Fisher Scientific, USA). Total P was determined using the
H2SO4-hydrogen peroxide hydrofluoric acid method (Wang et al.,
2020), and then the phosphorus in solution was determined by the
molybdenum-blue complex method (Murphy and Riley, 1962). Avail­
able phosphorus (AP) was tested by NH4F–HCl extraction method (Kuo
et al., 1988). The organic matter was Determined by potassium di­
chromate sulfuric acid heating method (Bao, 2000). Soil pH was
Fig. 3. Device diagram of stirring flow chamber experiment.
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Journal of Cleaner Production 347 (2022) 131202
measured by a pH meter in an aqueous suspension at a soil: water ratio
of 1: 2.5 w/v (Dai et al., 2017). The particle size analysis was measured
with pipette method (Deng et al., 2020). The soil surface positive charge
was determined by a modified Schofield method (Xu et al., 2003). The
specific surface area (SSA) was determined by the PSC method (Sun
et al., 2020).
2.3. Phosphorus sorption-desorption by stirred flow experiment
As shown in Fig. 3, a Polymethyl methacrylate reactor (25 cm3) is
used, and connected to a micro peristaltic pump through a rubber hose.
A 0.45 mm filter membrane is placed in a specially designed interlayer to
keep the soil in the reaction. In the reaction chamber, 2.50 g of the soil
sample and 25 ml of a reaction solution with a phosphorus concentration
of 100 mg/L (prepared from KH2PO4) containing 0.01 mol/L KCl was
placed, and repeat each sample three times. (Statement: The pH was not
controlled during the adsorption-desorption tests. TL soil pH increased
from 4.71 to 5.34 during the adsorption process, and then gradually
increased to 6.26 during the desorption process. LL soil pH increased
from 4.67 to 5.17 during the adsorption process, and then gradually
increased to 6.20 during the desorption process. SL soil pH increased
from 4.88 to 5.56 during the adsorption process, and then gradually
increased to 6.39 during the desorption process.)
T. Sun et al.
The input constant flow rate (jw) of the reaction solution is 1.0 mL/
min, and the suspension in the reaction chamber is continuously stirred
for 300 min with a magnetic stirrer. After the adsorption test is over, the
0.01 mol/L KCl solution is used to perform the desorption test for 300
min at the same flow rate as the adsorption process. The solution
collected from the reactor at 2 min intervals was then colorimetrically
tested for phosphorus concentration. The adsorption amount of P is
described by equation (1), according to López-Periago et al. (2008).
{ }
∑i [ ]
qa (ti) =
(C1 (j) − C2 (j))Δtjw
+ [C1 (i + 1) − C2 (i + 1)]
Ve
(1)
j=1
Ve m increase in phosphorus level of the cultivated soil after fertilization, and
where qa (ti) is the cumulative amount of adsorption at time (ti); C1(j)
and C2(j) are the concentration of phosphorus in the jth output solution
sample in the absence and presence of soil. And C1(i)) and C2(i) are the P
concentration in the chamber in the presence and absence of soil; Ve is
the effective volume of the solution in the reactor; m is the mass of the
soil sample. The desorption amount of P can be described by equation
(2).
{
i [ ] }
∑ (C2 (j) − C1 (j))Δtjw Ve
qd (ti) = + [C2 (i + 1) − C1 (i + 1)] (2)
j=1
V e m level (p < 0.05). The experiment data was treated statistically by using
where qd (ti) is the cumulative amount of desorption at time (ti).
The cumulative loss of Fe and Al ions carried by the solution during
the adsorption and desorption of the same sample can be described by
Eq. (3).
{
∑i ( ) }
C(j)Δtjw Ve
q(ti) = + C(i + 1) (3)
j=1
Ve m
where q (ti) is the cumulative loss of iron or aluminum ions at time (ti); C
(j) is the concentration of iron or aluminum ions in the jth output so­
lution sample in the presence of soil. And C(i) is the concentration of
iron or aluminum ions in the reaction chamber in the presence of soil.
2.4. Adsorption-desorption kinetic analysis and parameter calculation
To describe the adsorption and desorption kinetics of P, two types of
reaction sites are considered (Fernandez-Calvino et al., 2015b), and the
pseudo-first-order equations described by Fernandez-Calvino et al.
(2015a). (Eq (4) and (5)):
dq / dt = k1 (Fqmax − q) for q < qF (4)
dq / dt = k2 [(1 − F)qmax − q] for q ≥ qF (5)
where dq/dt is the adsorption or desorption rate (mg⋅kg− 1⋅min− 1), k1 is
the adsorption or desorption rate constant of the fast reaction site
(min− 1), and k2 is the adsorption or desorption rate related to the slow
reaction site constant (min− 1), F is the proportion of fast reaction sites
(mg⋅kg− 1), qmax is the maximum adsorption or desorption capacity (mg
kg− 1), q is the concentration of P adsorbed or desorbed (mg⋅kg− 1), qF is
the concentration of P adsorbed or desorbed at the transition from the
fast reaction site to the slow (mg⋅kg− 1). The previous equation can be
replaced by a linear change of dq/dt and qa, qd, or a composite curve of
two lines, where qF corresponds to the intercept. F is the ratio of qF/qmax.
If F = 1, the model is consistent with a pseudo first-order equation
(equation (4)) for a reaction site (Guedes et al., 2016).
2.5. Soil phosphorus loss prediction method and establishment of soil
phosphorus loss standard curve
After obtaining the accumulation curve (2.3) of the amount of
phosphorus absorbed with the flow time, in theory, the flow time can be
controlled to achieve the goal of adding a specific amount of phosphorus
to the soil sample, which can be used to simulate the process of
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Journal of Cleaner Production 347 (2022) 131202
increasing the soil phosphorus value after fertilizer application. With
reference to the adsorption curve equation, we set different flow times
corresponding to different phosphorus adsorption increments. After the
adsorption is completed, the soil phosphorus desorption experiment
(2.3) is carried out immediately. Finally, we obtain the phosphorus loss
value (desorbed phosphorus) of the same soil under different phos­
phorus simulation increment (absorbed phosphorus)conditions, and fit
the soil phosphorus loss standard curve accordingly. Generally speaking,
the standard curve of phosphorus loss is obtained by collecting undis­
turbed soils with lower phosphorus levels for experiments. Then test the
substitute it into the soil phosphorus loss standard curve. From this soil
phosphorus loss prediction method, the predicted value of soil phos­
phorus loss in this area can be calculated.
2.6. Statistical analysis
All determinations were made in triplicate and the standard devia­
tion is calculated. Pearson correlation was performed to determine the
relationship between adsorption-desorption parameters (qamax and
qdmax) and soil properties. All data were analyzed at a 95% confidence
the SPSS Version 22.0 software package. Curve fitting and charting were
performed using the SigmaPlot 14.0 software package.
3. Results
3.1. Adsorption and desorption of phosphorus in stirred flow chamber
experiments
With the change of reaction time (t), the accumulated adsorption and
desorption results of the three soils have significant differences (Fig. 4).
TL soil showed the highest P adsorption capacity, followed by LL and SL,
with qmax ranging from 520.1 to 865.7 mg kg− 1. From Fig. 4(a), it can be
seen that in SL and LL, most of the P has been adsorbed within the first
200 min of the reaction. For TL soil, this process mainly occurs within
the first 250 min of the reaction. This result reflects that the three soils
have different levels of affinity and adsorption capacity for phosphorus.
In the three soils, the desorption capacity of P is much smaller than
the adsorption capacity. The order of adsorption and desorption qmax is:
SL < LL < TL (Fig. 4, Table 2). The difference between the adsorption
capacity and desorption capacity characterizes the irreversibility and
hysteresis of adsorption. The ratio of desorption capacity to the
adsorption capacity (Dr) observed in TL soil is the smallest, and the
proportion of undesorbed phosphorus is about 55%. The Dr in SL and LL
soil is relatively large, and the proportion of undesorbed phosphorus is
about 47%.
The author’s previous batch experiment results of phosphorus
showed that, under the same phosphorus concentration (about 100 mg/
L), the order of the adsorption maximum (qamax) of the three erosive
weathered granite soils is TL > LL > SL, 420.4 mg/kg, 351.1 mg/kg,
222.8 mg/kg respectively. In contrast, the qmax values of the three types
of soils (TL, LL, SL) in the mixed flow experiment results under the same
phosphorus concentration increased by about 106%, 85%, and 133%
respectively. The qmax values of the three soils all increased significantly,
of which the LL value increased the least, and the SL increased the most.
The order of Dr is SL > TL > LL, approximately 0.24, 0.18, and 0.16.
In contrast, the Dr values of the three soils (TL, LL, SL) in the mixed flow
experiment results increased by about 150%, 231%, and 121% respec­
tively, under the same phosphorus concentration. The Dr value of the
three soils all increased significantly, of which LL increased the most,
and the increased Dr value of LL soil were close to SL soils.
The coefficient of variation of TL soil adsorption accumulation is
0.03–0.31, and the coefficient of variation of desorption accumulation is
0.11–0.32. The coefficient of variation of LL soil adsorption accumula­
tion is in the range of 0.14–0.28, and that of desorption accumulation is
T. Sun et al. Journal of Cleaner Production 347 (2022) 131202

Fig. 4. Comparison of the variation of phosphorus adsorption and desorption in three soil layers with time.

Table 1
Basic physicochemical properties of the three soil layers.
Layer Clay BD SSA TP AP SOM Fe Al Fea Ala pH Positive charge
(%) (g⋅cm− 3) (m2⋅g− 1) (g⋅kg− 1) (mg⋅kg− 1) (g⋅kg− 1) (g⋅kg− 1) (g⋅kg− 1) (g⋅kg− 1) (g⋅kg− 1) (cmol⋅kg− 1)

pH = Soil
7 pH

TL A 19.0 1.4 9.3 2.2 114.0 5.5 48.6 107.1 2.70 6.57 6.17 17.16 13.98
B 20.3 1.5 9.3 1.9 102.2 4.8 45.2 113.8 2.20 7.26 5.77 16.91 14.83
C 23.2 1.5 9.8 1.8 97.1 4.3 35.3 104.4 1.73 6.75 5.43 17.45 14.22
D 24.1 1.5 10.0 1.7 88.5 3.7 31.8 102.3 1.75 6.80 5.51 16.64 14.01

LL A 11.6 1.5 7.0 1.5 105.7 10.9 39.2 115.5 2.30 6.39 4.56 19.94 15.86
B 11.7 1.6 7.4 1.6 81.7 2.6 39.8 114.6 2.55 5.91 4.26 17.59 16.45
C 10.2 1.6 7.0 1.4 82.2 2.4 37.2 115.3 2.11 6.23 4.08 18.84 16.81
D 11.0 1.7 7.1 1.3 79.3 1.5 35.5 112.7 2.08 6.44 4.12 18.40 16.28

SL A 8.7 1.4 6.6 0.5 15.8 11.8 43.3 100.0 2.26 2.23 6.02 15.65 13.26
B 8.2 1.5 6.4 0.3 7.2 3.0 44.1 97.7 2.05 1.87 6.14 14.85 13.75
C 7.7 1.6 6.3 0.3 9.1 2.9 40.3 99.3 1.85 1.96 6.28 13.56 14.07
D 8.3 1.7 6.4 0.4 11.7 0.9 40.9 99.1 1.76 2.58 6.45 13.37 12.19

Note: SL-Sand layer; LL-Laterite layer; TL-Tillage layer; A-(0–15 cm), B-(15–30 cm), C-(30–45 cm), D-(45–60 cm); SSA-Specific surface area; SOM-Soil organic matter;
Fea, Ala-The amorphous Fe(Fe2O3) and Al(Al2O3); pH = 7, soil pH—the suspension pH when measuring the positive charge.

exhibits two types of adsorption sites with two different stages

Table 2
(Figs. 5–6, Table 2). The first stage shows that the reaction process takes
Kinetic parameters of adsorption and desorption of three soils.
place at a fast site, which is characterized by a significant decrease in the
Adsorption qF F qmax k1 k2 R1 2 R22 rate of adsorption and desorption (Figs. 5–6). The next stage is the result
TL 387.3 0.45 865.7 0.008 0.004 0.91 0.99 of the presence of the reaction at the slow site, and a significant decrease
LL 371.5 0.57 648.2 0.011 0.008 0.97 0.99 in the reaction rate is observed in the slow stage. The proportions (F) of
SL 359.9 0.69 520.1 0.0085 0.0061 0.97 0.94
the cumulative amount of the reaction at the fast sites of the three soils
Desorption qF F qmax k1 k2 R1 2 R22 are quite different (Table 2). In TL and LL, about half of the adsorption
TL 165.2 0.43 387.3 0.022 0.004 0.95 0.94 occurs at the fast sites, and the fraction of the fast sites (F) The ranges are
LL 227.3 0.67 341.4 0.021 0.012 0.97 0.98 0.45 and 0.57 respectively. The SL adsorption is lower (qmax = 520.1
SL 161.7 0.59 275.0 0.021 0.003 0.94 0.95 mg/kg) and occurs faster (F = 0.69).
Note: The above-mentioned parameters are obtained by averaging the LL soil and SL soil showed high and stable adsorption rate (Fig. 6),
adsorption-desorption results of the four mixed samples in each soil layer and and a high fast site fraction (F) (Table 2). In these two soils, the
analyzing them. qF: The concentration of P adsorbed or desorbed at the transi­ adsorption process mainly occurs in the short-term contact time with the
tion from the fast reaction site to the slow (mg⋅kg− 1); F: The proportion of fast phosphorus solution, and the rapid reaction is the main one. In the TL
reaction sites; qmax: Maximum adsorption or desorption capacity (mg⋅kg− 1); k1 soil, the reaction is more uniform, and the slow reaction is the main part.
and k2: The adsorption or desorption rate constant of the fast reaction site and The desorption rate of phosphorus is the fastest in LL soil, and the F
the slow reaction site constant, respectively (min− 1); R12 and R22: Determination value reaches 0.67. The F values of TL and SL are 0.43 and 0.59,
coefficients for the k1 and k2, respectively.
respectively (Table 3). The results show that for LL and SL soils, the
desorption occurs mainly at fast desorption sites, while the opposite is
in the range of 0.09–0.42. The coefficient of variation of the cumulative true for TL. The high desorption rate and final high desorption value of
amount of SL soil adsorption is 0.01–0.42, and the coefficient of varia­ LL may be caused by the loss of Fe and Al ions carrying phosphorus due
tion of the cumulative amount of desorption is 0.13–0.31. to its low soil pH. From Table 2, it can be ground, and the three soils are
in the adsorption-desorption stage. From the adsorption stage, k1, k2 all
3.2. Kinetic model of phosphorus adsorption-desorption in stirred flow satisfy SL > LL > TL ranking. For SL, its k1 parameter is 8.5 times and
chamber experiments 121.4 times that of LL and TL, and its k2 parameter is 7.6 and 15.3 times
that of LL and TL. From the desorption stage, the three soil parameters k1
The phosphorus kinetics described by the pseudo-first-order model

5
T. Sun et al. Journal of Cleaner Production 347 (2022) 131202

Fig. 5. Kinetic curves of phosphorus adsorption in three soil layers.

Fig. 6. Kinetic curves of phosphorus desorption in three soil layers.

Table 3
Correlation of phosphorus adsorption capacity with some selected soil properties.
Clay SSA TP AP SOM Fea Ala pH PC

pH = 7 At soil pH

qamax 0.86*** 0.89*** 0.91*** 0.85*** 0.23 0.35 0.79** − 0.04 0.50 0.15
qdmax 0.06 0.59* 0.75** 0.73** 0.54 0.63* 0.64* − 0.24 0.64* 0.36
Dr − 0.51 − 0.49 − 0.31 − 0.27 0.50 0.42 − 0.32 − 0.27 0.18 0.29

Note: SSA-Specific surface area; Fea, Ala-The amorphous Fe and Al; PC-Positive charge; SOM-Soil organic matter.
*** Significant at the 0.001 probability level.
** Significant at the 0.01 probability level.
* Significant at the 0.05 probability level.

is close, and the parameter k2 satisfies the level of LL > TL > SL. For LL,
its k2 parameter is 3 times and 4 times that of TL and SL. qdmax = 59.46TP− 1.33 AP+48.62SSA+113.59Fea− 26.71Ala+35.84PCpH = 7

R2 = 0.90 P = 0.023 (7)

3.3. The effect of soil physicochemical properties on phosphorus
adsorption and desorption
After fitting the soil physical and chemical data with the adsorption-
desorption results, we obtained the key factors affecting the phosphorus
adsorption and desorption process (Table 3). The key factors are clay
content, specific surface area, total phosphorus, available phosphorus,
amorphous iron, amorphous aluminum and positive soil charge (pH =
7). The fitting models (Eq (6) and Eq (7)) of adsorption capacity and
desorption capacity were obtained by calculation, R2 was 0.96 and 0.90,
respectively, and P value was 0.0004 and 0.023.
qamax = − 89.67 TP+6.27AP− 36.60Clay+238.65SSA− 75.28Ala
R2 = 0.96 P = 0.0004
Note: qamax、qdmax-The maximum adsorption or desorption capacity,
mg⋅kg− 1;TP-Total phosphorus, g⋅kg− 1; AP-Available phosphorus,
mg⋅kg− 1; Clay, %; SSA-Specific surface area, m2⋅g− 1; Ala、Fea-The
amorphous Fe and Al, g⋅kg− 1; PCpH = 7-The soil surface positive charge
at pH = 7, cmol⋅kg− 1.
3.3.1. Loss of iron and aluminum ions in stirred flow chamber experiments
Comparing the loss of iron ions, it is found that the loss of iron ions in
TL, LL, and SL are relatively similar, which are 52.7 mg/kg, 62.3 mg/kg,
and 52.6 mg/kg respectively (Fig. 7). With regard to the amount of
aluminum ion loss, the amount in TL and LL soils is similar, while the
amount in SL is significantly smaller. The amount of aluminum ion loss
in TL, LL, and SL is 1060.6 mg/kg, 811.5 mg/kg, 419.3 mg/kg
(6)

6
T. Sun et al.
Fig. 7. Comparison of Al and Fe ion loss over time.
respectively. Presumably, this result is mainly related to the original
content of amorphous Al, Fe and soil pH (Fig. 7, Table 1). In Fig. 7, the
first 400 min is the loss in the adsorption process, and 400–750 min is
the loss in the desorption phase.
3.4. Phosphorus loss standard curve
After fitting the data of phosphorus desorption at different adsorp­
tion stages, three standard curve of soil phosphorus loss were obtained.
After testing the increase and change of soil phosphorus within a certain
period of time, the maximum phosphorus loss from the soil under runoff
erosion conditions can be calculated through this standard curve.
Among the three models’ determination coefficients (R2), SL (R2 =
0.8831) soil is the largest, while TL (R2 = 0.8623) and LL (R2 = 0.8691)
are similar (Fig. 8).
4. Discussion
4.1. The effect of soil physical and chemical properties on phosphorus
adsorption and desorption
The highest qamax value obtained in the test corresponds to the TL soil
with the highest clay content. This index shows a significant correlation
at the level of 0.001 with a correlation coefficient of 0.86, confirming the
importance of clay for P adsorption. Previous studies rarely included soil
specific surface area in the phosphorus adsorption evaluation system
indicators, but the experimental results showed a high correlation (R =
0.89, p < 0.001), due to the smaller particle size of the clay component
(Sun et al., 2020). The presence of abundant aluminum compounds
often corresponds to a larger specific surface area, so this index has also
been included in the fitting model index system. Amorphous aluminum
shows a significant correlation with qamax and qdmax at the levels of 0.01
Fig. 8. Comparison of the three soils phosphorus loss standard curve.
7
Journal of Cleaner Production 347 (2022) 131202
and 0.05 respectively, and the correlation coefficients are 0.79 and 0.64
respectively. Amorphous iron also showed a higher correlation with
qdmax (R = 0.64, p < 0.05). The influence of amorphous aluminum and
iron is mainly due to the iron-aluminum oxide on the soil surface
forming surface precipitation or complexes with phosphate ions (Wei
et al., 2014; Weng et al., 2011; Werner et al., 2017).
The positive soil charge (pH = 7) is significantly positively correlated
with qdmax (R = 0.64, p < 0.05), which is exactly the opposite of the
batch experiments’ results (Sun et al., 2020). Differential pH and
iron-aluminum compound indicators are important reasons for the dif­
ference in soil positive charge (pH = 7) (Shamshuddin and Ismail,
1995). In the dynamic environment of stirring and flow, a large number
of reaction balances will shift to the left during the loss of iron and
aluminum ions in the later desorption experiment, leading to the
desorption of a large number of phosphate ions (Driscoll and Schecher,
1990; Wang et al., 2019). Therefore, there is a positive correlation in the
stirring flow experiment.
Soil total phosphorus and available phosphorus are important in­
dicators reflecting the initial soil phosphorus level. Both are significantly
positively correlated with qamax at the level of 0.001, and the correlation
coefficients are 0.91 and 0.85, respectively. These two indicators are
also significantly positively correlated with qdmax at the level of 0.01,
with correlation coefficients of 0.75 and 0.73. Under the same fertil­
ization level, soils with strong adsorption capacity can retain more
phosphorus. This law will be more obvious between soils with large
differences in adsorption capacity. This is also consistent with the pos­
itive correlation law of batch experiments. However, the initial phos­
phorus level is positively correlated to qdmax in the stirring flow test,
which is opposite to the negative correlation of the batch experiment.
The reason may be caused by the massive loss of aluminum ions and iron
ions during the desorption process of the stirred flow experiment.
There was no significant correlation between phosphorus adsorption
T. Sun et al.
capacity and soil organic matter (Table 3). We chose sloping land that
was not cultivated. Affected by humus and other factors, the SOM in the
top layer of the three soils was significantly higher than that in the
bottom soil. Among them, LL and SL soils’ top layer SOM is about 4–5
times that of the lower soil layer. The SOM of the TL top soil layer was
only 1.2–1.5 times that of the lower soil layer, and the TL top layer SOM
was even smaller than that of the LL and SL top layer. The reason for this
difference may be that fine particles such as clay can adsorb and fix
organic matter more tightly (Kaiser and Guggenberger, 2003; Smernik
and Kookana, 2015). However, in the study area with frequent rain­
storms, the soil on slopes is seriously eroded by rainfall, and the fine
particles in the top layer are greatly reduced with the runoff carried (Fu
et al., 2016). Therefore, the organic matter loss of the TL with the most
clay fine particles is more serious than that of the LL and the SL.
4.2. The influence of iron and aluminum ion loss on phosphorus
adsorption-desorption process
According to the results of 3.3.1, it can be seen that the loss of
aluminum and iron ions has a certain influence on the phosphorus
adsorption in the stirring flow experiment, and the influence of
aluminum ions is greater. The principle may be the double loss of
aluminum ions and phosphate ions during the desorption process,
causing the continuous balance of precipitation or other reversible re­
actions to shift to the left, which promotes the desorption of phosphate
ions.
The continuous dissolution and loss of iron and aluminum ions may
reduce some sites on the clay surface that cause phosphate ion adsorp­
tion (Abdala et al., 2015; Li and Guan, 2011). Lower soil pH makes this
effect more prominent in LL, so the increase in phosphorus adsorption
caused by LL soil in the stirred flow experiment is less (Antoniadis et al.,
2016). In the adsorption process, compared with the phosphorus batch
experiment, the consistent high adsorbent concentration in the reaction
chamber will effectively promote the phosphorus adsorption reaction.
Constant flow and renewal environment may cause the dissolution
and precipitation reaction to continue to move to the right, continuously
taking away a large amount of aluminum and iron ions, and the lost iron
and aluminum ions also cause a large amount of desorption of phos­
phorus ions. As a result, compared with the batch experiment, the
phosphorus desorption rate in the stirred flow experiment was
improved. It can be seen from Table 1 that the content of amorphous
iron and aluminum in LL soil is significantly higher than that in SL. The
clay content and pH caused the Dr in the batch experiment to be similar,
and the pH is now weakened. In the desorption process, compared with
the continuous and consistent zero adsorbent environment of the
phosphorus batch experiment in the reaction chamber, it will effectively
promote the desorption of phosphorus.
4.3. Phosphorus adsorption-desorption kinetics
Studies have shown that after phosphorus is adsorbed on the soil
surface, it will cover strong fast spots and relatively loose slow spots
(Rahutomo et al., 2018; Yin et al., 1997). The continuous desorption
process of zero adsorbent in the gradual flow experiment can promote
the rapid desorption of phosphorus attached to the slow site, which is
more in line with the actual phosphorus loss under the condition of high
fertilizer coverage in the field. The stages of P adsorption and desorption
are divided into two stages: fast and slow, which are similar to some of
the stirring flow adsorption-desorption experiments (Guedes et al.,
2016). In this experiment, in order to change the influence of the initial
solution volume limit on the initial stage of the reaction, the reaction
vessel is designed to be 25 cm3, and the initial reaction vessel is almost
filled with the solution. The peristaltic pump was turned on in advance,
and the soil sample was added when it was almost full and quickly close
the lid.
The slow adsorption sites in TL soil account for the main part. Since
8
Journal of Cleaner Production 347 (2022) 131202
the fast adsorption site and the slow adsorption site correspond to high-
affinity and low-affinity phosphorus sites respectively (Colombo et al.,
1994; Phillips, 2002), the small number of high-affinity phosphorus sites
during the adsorption reaction leads to the initial high-rate adsorption.
The increase of low-affinity phosphorous sites results in a very persistent
low adsorption rate in the late stage of the adsorption reaction. A large
number of low-affinity sites determine the overall higher phosphorus
release rate of TL soil desorption reaction, which is much higher than the
reaction rate of LL and SL soils in the same period. It may be due to the
difference in clay content and the deviation of the ratio, which makes
the influence of slow adsorption sites prominent (Lair et al., 2009). This
produces a high correlation between the adsorption-desorption results
and the clay content and ratio (Table 2).
The adsorption in LL and SL mainly occurs at fast adsorption sites.
During the adsorption reaction, both LL and SL soils accounted for a
large proportion of high-affinity phosphorus sites, leading to rapid
adsorption in the early stage of the reaction. Among them, LL is the
fastest, and SL has a lower initial rapid adsorption rate due to the lower
absolute number of phosphorus sites. Fewer low-affinity phosphorus
sites also determine the rapid end of the LL and SL soil adsorption re­
action. During the desorption process, the low-affinity phosphorous sites
accounted for a small proportion of LL and SL, which led to the initial
rapid release. In the later release process, the high-affinity sites
accounted for the main part of the sustained low-rate release. However,
there is a certain difference between LL and SL, and the rate of LL is
higher than that of SL. This is due to the abundant iron and aluminum
compounds in LL soil, the binding strength of high affinity sites corre­
lated positively with soil Fe-d, Al-o, Al-d, and crystalline iron oxide
contents (Fe-d-Fe-o) (Mehmood et al., 2010). Wang and Tzou (1995)
also reported that the amount of P-sorption was correlated with the free
iron oxide (Fe-d) contents of the magnetic clay fractions (r = 0.82).
Because the positively charged iron-aluminum compound attached to
the soil surface precipitates or complexes with phosphate ions (Gerard,
2016; Gypser et al., 2018), the early adsorption rate of TL and LL soil is
high, while the early adsorption rate of SL soil is relatively small.
Although the amorphous aluminum content of LL soil is lower than that
of TL, the pH value of the soil will result in a higher adsorption rate of
aluminum in LL soil than TL soil in the previous period, or it may be due
to the higher initial phosphorus in TL soil. The higher valence form
exists at the level, which enhanced the adsorption of phosphate anions.
The law of surface charge can explain the important role of amorphous
aluminum in the adsorption-desorption process from the electro­
chemical perspective. The higher adsorption rate of LL soil than TL soil
in the early stage may also be due to the higher initial phosphorus level
of TL soil occupying a certain strong adsorption of P adsorption sites
(Zhang et al., 2005). This can also explain that in the adsorption process
of TL soil, slow site adsorption accounts for the main adsorption ratio,
while the proportion of fast adsorption sites in LL and SL soils is grad­
ually increasing.
Among three soils, the proportion of fast desorption sites for LL is the
highest, which reflects that the adsorption capacity of P in LL soil is the
lowest and its accessibility is higher (Griffin and Jurinak, 1974). In LL
soils with more aluminum compounds, with the beginning of the
desorption process, the chemical reaction may shift to the left under the
conditions of continuous loss of aluminum and iron ions. Eventually,
more phosphate ions are desorbed. The F value of the desorption process
of SL soil is relatively large. This is because under the condition that the
clay content and the aluminum compound content exist simultaneously,
the weak adsorption sites of P on the surface of the SL soil account for the
majority. Therefore, the final desorption process of SL soil maintains the
previous high desorption rate. In the desorption process, a small F value
may reduce the desorption rate and increase the hysteresis in the soil.
4.4. Application prospects of phosphorus loss standard curve
After testing the soil phosphorus content after initial fertilization, the
T. Sun et al.
phosphorus loss can be calculated by substituting the soil phosphorus
content into the standard curve. The obtained phosphorus loss value is
the maximum phosphorus loss that can be brought to the soil by rain­
water runoff erosion during the subsequent fertilization interval. Based
on the establishment of the phosphorus loss standard curve, we can
calculate the maximum phosphorus loss of the entire area through the
soil phosphorus loss prediction method only by regularly collecting
typical soil samples in the area. It is recommended that the interval of
soil sampling is the fertilization cycle of the farmland.
In the actual application of this method, it is recommended to verify
and adjust the mixed flow standard curve obtained from the soil in the
area in combination with the experimental data of the artificial rain soil
pond in the past. This can make the predicted results more accurate and
credible, but at the same time it brings limitations for field conditions
(artificial rainfall simulation experiment).
In previous studies, the phosphorus loss value was generally ob­
tained through a large number of artificial rainfall simulation experi­
ments or field in-situ monitoring experiments (Wu et al., 2018; Zhang
et al., 2018). These research methods have limitations such as long
experimental periods and expensive platform construction costs. It is
difficult to carry out long-term continuous monitoring research in a
large area, and it is difficult to estimate the nutrient loss of soil flow. The
mixing flow-phosphorus loss standard curve proposed in this study can
avoid the shortcomings of the previous research methods, and can also
estimate the phosphorus loss in the soil. Applying the phosphorus loss
standard curve to the specific loss model and regional non-point source
pollution research is a direction with broad research and application
prospects. It can even be extended to predict the loss of other soil
pollutants.
5. Conclusion
The erosive weathered granite soil has a strong phosphorus fixation
effect. 53% of the phosphorus in the TL soil is not desorbed, and 47% in
the SL and LL soil. The kinetic characteristics of phosphorus in the
erosive weathered granite soil are highly related to the affinity of the
solid soil matrix, where a large amount of P is adsorbed within a short
time after the reaction starts. Most of the reactions in SL and LL soils
occur at fast sites, while in TL soils, they mainly occur at slow sites. The
key factors affecting the soil adsorption-desorption process are clay
content, specific surface area, total phosphorus, available phosphorus,
amorphous iron, amorphous aluminum and positive soil charge (pH =
7). The key related factors affecting phosphorus adsorption-desorption
can be used to fit the models for calculating the qamax and qdmax of soil
in erosive weathered granite area. The phosphorus loss standard curve
can realize a large-scale and long-term continuous monitoring and
research on phosphorus, and can become an important reference for
other soil pollutant loss prediction studies. This research can provide
theoretical basis and reference for phosphorus utilization in the phos­
phorus management of severely eroded soil in Zhejiang Province,
thereby improving phosphorus utilization and reducing soil phosphorus
loss.
Funding information
This work was supported by the National Natural Science Foundation
of China [Grant No. 41877065].
CRediT authorship contribution statement
Tianyu Sun: Conceptualization, Methodology, Writing – original
draft. Kai Fei: Software, Validation, Data curation. Longzhou Deng:
Investigation, Software, Supervision. Liping Zhang: Funding acquisi­
tion, Writing – review & editing. Xiaojuan Fan: Investigation. Yanhong
Wu: Investigation.
9
Journal of Cleaner Production 347 (2022) 131202
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
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