Sustainable Chemistry and Pharmacy 17 (2020) 100294

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Sustainable Chemistry and Pharmacy

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Optimization of silver recovery from waste X-ray radiographic films by

oxalic acid extraction with response surface methodology
Jaycee C. Urriquia , Pia Monique C. Rheinhardt , Nareija Najma T. Tanggol , Rontgen Gapusan ,
Mary Donnabelle L. Balela *
Sustainable Electronic Materials Group, Department of Mining, Metallurgical, and Materials Engineering, University of the Philippines, Diliman, Quezon City, 1101,
Philippines

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

Keywords: Waste X-ray radiographic films contain an appreciable amount of silver (Ag) that can be recovered and
Ag recovery reprocessed. Most of the existing methods of Ag recovery from waste radiographic films are expensive and
X-ray films harmful to the environment. In this study, the extraction of Ag from waste radiographic films was done using
RSM
oxalic acid solution heated at 90–100 ◦ C. XRD and SEM results reveal that the recovered residue contains pure
Box-behnken
metallic Ag spherical microparticles. According to the response surface methodology (RSM) based on three-level,
Oxalic acid
three-factorial Box-Behnken design, the optimized stripping conditions are oxalic acid concentration of 9.97% w/
v, extraction temperature of 99.51 ◦ C, and extraction time of 16.62 min. The predicted and actual % Ag recovery
are of 94.94 and 90.07%, respectively. Reusability study confirms that the oxalic acid solution can be reused for
several runs of Ag extraction. Initial Ag recovery of ~68.9% decreased to ~28.2% after 4 cycles of reusing the
extraction solution.

1. Introduction recovered (Aktas et al., 2010). Photography is still a large consumer of

Silver (Ag), one of the valuable and noble metals on Earth’s crust, has
numerous industrial and technological applications because of its
excellent photosensitivity, optical reflectivity, antibacterial activity, and
thermal and electrical conductivities (Bas et al., 2012; Engidayehu and
Sahu, 2020; Wei et al., 2015). For example, Ag nanoparticles were re­
ported to display excellent antimicrobial property against E. coli and
S. aureus (Cho et al., 2005). In another work, Ag nanoparticles prepared
by electroless deposition were sintered at room temperature and dis­
played potential as conductive ink (Rezaga and Balela, 2018, 2020;
Corsino and Balela, 2017). Ag nanowires, on the other hand, have been
employed in the development of flexible transparent touch panel
because of their excellent electrical conductivity and mechanical prop­
erty (De Guzman et al., 2018; de Guzman and Balela, 2017). Due to the
high Ag consumption worldwide, the depletion of the primary sources of
Ag is inevitable.
The extraction and recovery of Ag from Ag-containing waste mate­
rials has become necessary. It was reported that 25% of the global de­
mand of Ag is supplied by recycling, and photographic wastes represent
75% of the total volume of Ag-containing waste materials being
Ag in the form of silver halide crystals, such as silver bromide (AgBr) and
silver iodide (AgI) (Bas et al., 2012; Engidayehu and Sahu, 2020).
Among the photographic films, X-ray radiographic films has the highest
amount of Ag, and about 5–15 g Ag is used to prepare 1 kg of X-ray
radiographic film (Engidayehu and Sahu, 2020; Abdel-Aal and Farhaly,
2007).
In general, metal extraction from metal-containing waste materials
can be done by pyrometallurgical or hydrometallurgical processes
(Abdel-Aal and Farhaly, 2007). Pyrometallurgical processes, in which
the source waste materials are subjected to incineration, are expensive
due to the high energy requirement. Main disadvantages of these pro­
cesses also include emission of toxic gases and low recovery of metal
(Havlik et al., 2010; Ojeda et al., 2009). On the other hand, hydromet­
allurgical processes, which typically involve leaching as the first step,
are relatively economical with high yield (Bas et al., 2012; Abdel-Aal
and Farhaly, 2007; Garcia, 1986; Nakiboglu et al., 2003; Zhouxiang
et al., 2008; Arslan et al., 2011). The hydrometallurgical extraction of
Ag from X-ray radiographic films has been investigated using various
reagents including nitric acid (Abdel-Aal and Farhaly, 2007; Nakiboglu
et al., 2003; Arslan et al., 2011), sodium cyanide (Garcia, 1986), sodium

* Corresponding author.
E-mail address: mlbalela1@up.edu.ph (M.D.L. Balela).

https://doi.org/10.1016/j.scp.2020.100294
Received 5 March 2020; Received in revised form 1 July 2020; Accepted 4 July 2020
Available online 13 August 2020
2352-5541/© 2020 Elsevier B.V. All rights reserved.
J.C. Urriquia et al. Sustainable Chemistry and Pharmacy 17 (2020) 100294

hydroxide (Nakiboglu et al., 2003; Zhouxiang et al., 2008; Arslan et al., Table 1
2011), ferric chloride (Nakiboglu et al., 2003; Masebinu and Muzenda, Box-Behnken design matrix for the Ag extraction conditions and the corre­
2014), oxalic acid (Arslan et al., 2011; Masebinu and Muzenda, 2014; sponding experimental and predicted Ag recovery.
Syed et al., 2002; Khunprasert et al., 2008), malonic acid (Khunprasert Runs Oxalic acid Extraction Extraction Yexperimental Ypredicted
et al., 2008) and acetic acid (Khunprasert et al., 2008). concentration temperature time (min) (%) (%)
It was reported that sodium cyanide solution could recover the Ag (% w/v) (◦ C)

content from X-ray radiographic films with an almost 100% yield 1 1 90 10 2.39 4.15
(Garcia, 1986). However, the high toxicity of the reagent is a great 2 10 90 10 48.16 45.28
3 1 100 10 17.38 20.39
drawback for this method. On the other hand, nitric acid solution at high
4 10 100 10 79.15 77.27
normality can also extract about 100% of Ag from radiographic films 5 1 95 5 0.0 2.94
(Abdel-Aal and Farhaly, 2007; Zhouxiang et al., 2008). However, the 6 10 95 5 30.73 38.80
process also produces nitrogen oxides, which are one of the major air 7 1 95 20 20.93 13.22
pollutants (Abdel-Aal and Farhaly, 2007; Zhouxiang et al., 2008). 8 10 95 20 91.82 88.51
9 5 90 5 0.0 − 4.76
Moreover, the Ag products obtained using cyanide and nitric acid are in 10 5 100 5 17.79 11.53
the form of Ag complexes (i.e. silver cyanate and silver nitrate). Thus, 11 5 90 20 6.73 12.61
additional process, such as electrolysis, is required to recover Ag as pure 12 5 100 20 44.63 49.76
metal (Khunprasert et al., 2008). It was also demonstrated that oxalic 13 5 95 10 18.67 23.11
14 5 95 10 26.7 23.11
acid solution can efficiently extract about 90–100% of Ag from radio­
15 5 95 10 23.97 23.11
graphic films (Syed et al., 2002; Khunprasert et al., 2008). Compared to
leaching reagents such as cyanide and nitric acid, oxalic acid is relatively
environment-friendly. In addition, the recovered Ag particles are in their variance (ANOVA), coefficient of determination (R2), and response
metallic form without any side reaction, e.g. formation of complexes surface plots using the said software. The relationships of the indepen­
with oxalic acid (Khunprasert et al., 2008). dent variables with the responses were established by fitting the data
In this study, the extraction of Ag from X-ray radiographic films was points into the following second-order polynomial equation:
carried out via stripping process using oxalic acid. Response surface
methodology (RSM) based on three-level, three-factorial Box-Behnken Y predicted = β0 + Σβi Xi + Σβii X 2i + Σβij Xi Xj + ε (1)
experimental design was employed to optimize the Ag extraction pa­
where Ypredicted represents the predicted Ag recovery, β0 is the constant
rameters, namely, oxalic acid concentration, extraction temperature,
coefficient, βi is the ith linear coefficient of the input factor Xi (i = 1 −
and extraction time. A second-order polynomial regression model was
3), βii is the ith second order coefficient of the input factor Xi , βij is the
used to investigate the effects of the interactions between the extraction
parameters. Finally, the reusability of the oxalic acid solution for mul­ coefficient of the interaction between the input factors Xi and Xj (j = 1 −
tiple stripping runs was determined. 3, i ∕
= j), and ε is the error of the model [21].

2. Methodology 2.3. Characterization

2.1. Materials
Waste radiographic films were acquired from the Pacific Royal Basic
Food Products Inc, Candelaria, Quezon, Philippines. Oxalic acid
(COOH2⋅2H2O, 99.5%) and nitric acid (HNO3, 50.0%) were purchased
from Techno Pharmchem, New Delhi, India and Sigma-Aldrich,
Singapore, respectively. Distilled water was used for acid solution
preparation and rinsing.
2.2. Silver extraction and optimization of extraction conditions
The waste radiographic films were cut into small pieces (2 cm × 2
cm). The film pieces (50 g) were placed in 100 mL 1–10% w/v oxalic
acid solution. The extraction of Ag was carried out by heating the so­
lution at 90–100 ◦ C for 5–20 min. The stripping of Ag was indicated by
the change in the X-ray film color from black to clear. The clear polyester
films were removed from the stripping solution and then placed in
boiling water at 100 ◦ C for about 10 min to completely separate the Ag-
containing solids on the surface. The solid residues from the used
stripping solution and used hot water for washing the clear polyester
films were filtered. Afterwards, the residues were dried at 110 ◦ C
overnight. The residues were then heat-treated at 550 ◦ C for 2 h in air to
decompose any organic matter and recover the Ag metal. After heat-
treatment, the final weight of the residue was obtained.
The optimization of the Ag extraction was performed using three-
level, three-factorial Box-Behnken experimental design. The oxalic
acid concentration, extraction temperature, and extraction time were
used as the independent input variables. The Ag recovery was taken as
the response. The experimental design matrix shown in Table 1 was
obtained using a Design Expert 12 software (Stat-Ease Inc. Minneapolis,
USA). The experimental data were analyzed by applying the analysis of
The average Ag content of the waste radiographic films was deter­
mined by acid digestion of 10 g waste X-ray films in 20 mL concentrated
HNO3 (15.8 M) at 100 ◦ C for 10 min. Afterwards, the clear polyester
films were removed and washed. The acid solution, with the washing
solution, was diluted to 50 mL for elemental testing. The amount of
leached Ag in the acid solution was determined by X-ray fluorescence
spectrometer (XRF, XOS HD Mobile). The morphology and crystal
structure of the recovered Ag-containing residues after heat treatment
were investigated using a JEOL JSM 5310 scanning electron microscope
(SEM) and a Shimadzu XRD-7000 X-ray diffractometer (XRD),
respectively.
3. Results and discussion
3.1. Determination of the initial Ag content of waste radiographic films
The Ag content of the radiographic films was determined by acid
digestion using concentrated HNO3. The following chemical reaction
describes the dissolution of Ag by HNO3:
3 Ag(s) + 4HNO3(aq) → 3AgNO3(aq) + 2H2O(l) + NO(g) (2)
The complete decoloration of the films to a yellowish clear polyester
film (Fig. 1) indicates the complete removal of Ag from the films during
acid digestion. It is also clear from the image that the polyester films
were not dissolved during acid digestion. As listed in Table 2, the weight
of Ag per ~10 g radiographic film was found to be in the range of
0.1691–0.2074 g, which is equivalent to 1.69 to 2.06 wt %, respectively.
3.2. Extraction of Ag using oxalic acid solution
Preliminary Ag extraction was performed using 10% w/v oxalic acid

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J.C. Urriquia et al. Sustainable Chemistry and Pharmacy 17 (2020) 100294

Fig. 1. Image of X-ray radiographic films after acid digestion with HNO3.
Fig. 2. XRD spectrum of the Ag-containing residue recovered after heat treat­
ment at 550 ◦ C for 2 h.
Table 2
Ag content of waste X-ray radiographic films determined by acid digestion.
Sample Initial film weight, WX- Weight of Ag, WAg Ag content per WX-ray
ray (g) (g) (%)

1 10.004 0.1691 1.690

2 10.076 0.1790 1.777
3 10.082 0.2074 2.057

heated at 100 ◦ C for 20 min. Black residues were obtained after the
reaction. The polymer substrates were also completely decolorized,
which results to transparent yellowish films. After filtration, both the
residue and filtrate were subjected to XRF analysis to determine the
amount of Ag present in ppm or mg/L. Ag concentrations of 42.60 and
418.25 ppm were measured from the oxalic acid filtrate and Ag-
containing residue, respectively. Typically, radiographic films are
composed of polyester film that serves as the flexible substrate material,
an emulsion layer of gelatin, and dispersed silver halide crystals. During
the reaction, the oxalic acid possibly dissolves the gelatin by breaking
down its cross-link network (Khunprasert et al., 2008). As a result, the
Ag-containing residues are released into the solution in the form of a
sludge (Khunprasert et al., 2008). After heat treatment at 550 ◦ C, the Fig. 3. Corresponding SEM image of the Ag-containing residue recovered after
appearance of the obtained Ag-containing residues is similar to that of a heat treatment at 550 ◦ C for 2 h.
pure Ag metal powder.
Fig. 2 shows the X-ray diffraction pattern of the Ag powder obtained
3.3. Optimization of the Ag extraction parameters
after heat treatment of the Ag-containing residues at 550 ◦ C. The strong
and narrow diffraction peaks located at 2θ = 37.82◦ , 44.00◦ , 64.12◦ ,
The corresponding experimental and predicted Ag recovery are
77.04◦ and 81.17◦ correspond to the reflections of the (111), (200),
summarized in Table 1. The highest Ag recovery of about 91.82% was
(220), (311) and (222) planes of metallic Ag crystal, respectively (Aktas
achieved using 10% w/v oxalic acid at an extraction temperature of 95
et al., 2010). The sharpness of the XRD peaks indicate the high crys­ ◦
C for 20 min. In fact, about 30.73% Ag were already recovered after 5
tallinity of the Ag powder. In addition, no peaks attributed to the pres­
min at an oxalic acid concentration of 10% w/v. On the other hand,
ence of Ag compounds, such as silver oxide and silver oxalate, were
lower Ag recoveries of 20.93 and 44.63% were obtained using 1 and 5%
observed. This suggests that the final product after heat treatment was
w/v oxalic acid, respectively, even at longer reaction time (20 min).
pure Ag powder.
Results suggest that the extraction of Ag from the radiographic film was
The corresponding SEM micrograph of the recovered Ag powder is
favorable at the highest concentration of oxalic acid. Furthermore,
shown in Fig. 3. It can be observed that spherical Ag microparticles were
higher amount of Ag was also recovered at longer time of extraction.
obtained after heat treatment. It was reported that the Ag particles
The following second-order polynomial equation, which describes
suspended in the gelatin layer of the processed X-ray films were spher­
the empirical relation between the response and independent variables
ical in shape (Khunprasert et al., 2008). Hence, result suggests that the
in terms of coded units, was obtained from the experimental results in
Ag particles maintained their shape after the extraction process with
Table 1:
minimal dissolution in the oxalic acid solution. This is further supported
by the low concentration of Ag determined from the filtrate after sepa­
ration of the residue.

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J.C. Urriquia et al. Sustainable Chemistry and Pharmacy 17 (2020) 100294

Ypredicted = 24.2234 + 25.8193X1 + 8.0385X2 + 12.3888X3

+ 1.9687X1 X2 + 9.8577X1 X3 + 2.6076X2 X3 (3)
+ 13.3798X1 2 − 0.5701X2 2 − 9.2016X3 2

where X1 , X2 and X3 represent the oxalic acid concentration, extraction

temperature, and extraction time, respectively. The signs and magni­
tudes of the coefficients can provide insights on how the independent
variables influence the response (Perez et al., 2017). Positive coefficients
indicate positive effect on the response, while negative ones correspond
to the opposite effect. As seen in Eq. (3), all the independent factors, i.e.
oxalic acid concentration, extraction temperature, and extraction time,
have positive effect on the recovery of Ag. Moreover, the coefficient of
X1 has the highest magnitude, which signifies that the oxalic acid con­
centration has the highest influence on the recovery of Ag.
The analysis of variance (ANOVA) was applied to determine the
statistical significance and adequacy of the obtained second-order
polynomial regression model (Perez et al., 2017; Zhu et al., 2014).
The ANOVA results are summarized in Table 3. High F-values and low
p-values (i.e. p < 0.05) suggest the significance of the model terms,
while p > 0.1 suggests that the terms are insignificant. With a model
F-value of 17.30, analysis suggests that the model is statistically signif­
icant, and there is only 0.29% chance that the F-value is caused by noise.
As seen in Table 3, the terms X1, X2, X3 and X21 are also statistically
significant. This supports the earlier analysis that all the input variables
would influence the response. Variable X1 also has the lowest p-value
(highest F-value), which confirms that the oxalic acid concentration has
the most significant effect on the extraction of Ag among the indepen­
dent factors. The lack-of-fit F-value of 5.82 implies the insignificance of
the lack-of-fit relative to the pure error (Perez et al., 2017). Therefore,
the second-order polynomial model could be used as a reliable predictor
of Ag recovery.
The coefficient of determination R2 was used to analyze the corre­
lation between the experimental (Yexperimental) and predicted (Ypredicted)
Ag recoveries (Liu et al., 2012). With an R2 value of 0.9689, the
experimental data are in good agreement with the predicted responses
as shown in Fig. 4, where the data points are distributed almost along a
straight line. The adjusted R2 also evaluates the goodness of a fit, while
correcting the R2 for the sample size and number of terms in the model
by using the degrees of freedom during the calculation (Perez et al.,
2017; Zhu et al., 2014). The adjusted R2 value (0.9129) also confirms
that model is of high significance. Lastly, the adequacy precision mea­
sures the signal to noise ratio, and an obtained ratio of 14.183 (should
be > 4) indicates the adequacy of the signal (Perez et al., 2017; Zhu
et al., 2014; Liu et al., 2012).
The response surface plots can provide important information
regarding the effects of each independent variable, as well as their in­
teractions with each other, on the response (Zhu et al., 2014). Fig. 5
shows the generated 3D surface response plots for each two-variable
interaction. It can be confirmed that all the independent factors
Fig. 4. Plot of the predicted and experimental Ag recoveries.
influenced the amount of Ag recovered from the waste radiographic
films. The Ag recovery improves as the values of the independent factors
were increased. In addition, the oxalic acid concentration has the
greatest effect on the amount of Ag recovered. These plots validate the
findings from the previous statistical analyses. The effect of the inter­
action between the oxalic acid concentration and extraction tempera­
ture at a constant extraction time of 20 min is shown in Fig. 5a. The
extraction of Ag could only take place when the oxalic acid concentra­
tion and extraction time were set to at least ~2.5% w/v and ~91 ◦ C,
respectively. Complete Ag recovery could be achieved either with 10%
w/v oxalic acid at ~98 ◦ C or ~9.4% w/v at 100 ◦ C. The increase in the
recovery is attributed to the increase in the extraction strength of the
oxalic acid solution at higher temperature (Khunprasert et al., 2008).
Fig. 5b shows the effect of the interaction of oxalic acid concentra­
tion and extraction time at a constant temperature of 100 ◦ C. With 1%
w/v oxalic acid, Ag extraction already occurred in 5 min with Ag re­
covery of ~5.5%. A maximum recovery of ~26.2% was achieved in 20
min. On the other hand, with 10% w/v oxalic acid, 49% was recovered
during the first 5 min of extraction, while a complete recovery was
achieved in ~16 min. This suggests that a sufficient amount of time was
needed to completely dissolve the emulsion layer and liberate all the Ag
particles. On the other hand, Fig. 5c shows the effect of the interaction
between the extraction temperature and extraction time at a constant
oxalic acid concentration of 10% w/v. At 90 ◦ C, minimum and
maximum Ag recoveries of ~24.1 and ~63.4% were achieved in 5 and
20 min of extraction, respectively. Again, at the oxalic acid

Table 3
ANOVA results for the obtained second-order polynomial regression model.
Source Sum of Squares df Mean F-value p-value

Model 10098.21 9 1122.024 17.29627 0.002942 significant

X1-Oxalic acid concentration 3441.981 1 3441.981 53.05899 0.000763
X2-Extraction temperature 640.8248 1 640.8248 9.878473 0.02558
X3-Extraction time 829.8262 1 829.8262 12.79198 0.015932
X1X2 62.37553 1 62.37553 0.961534 0.371834
X1X3 412.6946 1 412.6946 6.361789 0.053028
X2X3 114.8029 1 114.8029 1.769716 0.240863
X21 641.1169 1 641.1169 9.882976 0.025559
X22 19.19453 1 19.19453 0.295888 0.609839
X23 234.9615 1 234.9615 3.62199 0.115396
Residual 324.3542 5 64.87084
Lack of Fit 291.0129 3 97.00431 5.818874 0.150156 not significant
Pure Error 33.34127 2 16.67063
Cor Total 10422.57 14

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J.C. Urriquia et al. Sustainable Chemistry and Pharmacy 17 (2020) 100294

Fig. 5. 3D response surface plots of the effects of (a) oxalic acid concentration and extraction temperature, (b) oxalic acid concentration and extraction time, and (c)
extraction temperature and time interactions.

concentration and extraction temperature of 10% w/v and 100 ◦ C,

Table 4
respectively, it would take at least ~16 min to completely extract all the
Reusability experimental setup and the corresponding Ag recovery for each run.
Ag from the radiographic films.
According to the second-order polynomial regression model, as Run Initial weight of Oxalic acid Amount of Ag Ag recovery
X-ray films (g) solution volume recovered (g) (%)
calculated from the Design Expert software, several possible combina­ (mL)
tions of optimum values were obtained. The following set of extraction
1 100 200 1.84 65.95
conditions is among the 100 combinations of optimum values: oxalic
2 50 100 0.92 50.31
acid concentration of 9.97% w/v, extraction temperature of 99.51 ◦ C, 3 25 50 0.46 39.76
and extraction time of 16.62 min. However, in reality, it is more 4 12.5 25 0.23 28.21
convenient to set the oxalic acid concentration, extraction temperature,
and extraction time to 10% w/v, 100 ◦ C, and 17 min, respectively.
run was decreased to keep the solid to liquid ratio constant. From an
initial Ag recovery of ~65.9% during the first extraction run, it consis­
3.4. Reusability of the oxalic acid solution
tently dropped to ~28.2% until the fourth run. The reduction in the
extraction efficiency could be due to the presence of impurities in the
The reusability of the extracting solution was performed by using the
stripping solution. Elemental analysis of the stripping solution indicates
same oxalic acid solution for four extraction runs. For each extraction
the presence of Ag, Ca and K. Ag is possibly from tiny Ag particles that
run, the oxalic acid concentration, extraction temperature and time
remained in the solution. On the other hand, Ca and K could be from the
were set to 8.7% w/v, ~92 ◦ C and ~20 min, respectively. The experi­
developer and fixing solutions. In addition, some gelatin is possibly
mental setup and the corresponding Ag recovery are shown in Table 4.
present in the used oxalic acid solution. Nonetheless, results confirm
Losses in the amount of oxalic acid solution were incurred after each
that the solution could be reused for few consecutive extraction runs.
extraction run. Thus, the initial amount of waste X-ray films utilized per

5
J.C. Urriquia et al.
4. Conclusion
The recovery of Ag from waste X-ray radiographic films were easily
carried out via extraction using oxalic acid solution at near boiling point.
Material characterizations revealed that the recovered residue after heat
treatment was pure Ag metal powder, which was composed of spherical
microparticles. Response surface methodology coupled with the Box-
Behnken experimental design was applied to optimize the extraction
conditions. According to the statistical analyses and response surface
plots, one of the optimum sets of extraction conditions are oxalic acid
concentration of 9.97% w/v, extraction temperature of 99.51 ◦ C, and
extraction time of 16.62 min. A more convenient set of optimum con­
ditions is given by: oxalic acid concentration of 10% w/v, extraction
temperature of 100 ◦ C, and extraction time of 17 min. Finally, it was
demonstrated that the oxalic acid solution could be reused for several
extraction runs.
CRediT authorship contribution statement
Jaycee C. Urriquia: Writing - original draft. Pia Monique C.
Rheinhardt: Writing - original draft. Nareija Najma T. Tanggol:
Writing - original draft. Rontgen Gapusan: Writing - original draft,
Formal analysis. Mary Donnabelle L. Balela: Supervision, Writing -
review & editing.
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.
Acknowledgment
The authors would like to express their gratitude to the College of
Engineering, University of the Philippines, Diliman, Quezon City for the
financial support under the Don Mustaffa Loong Thesis grant. Dr. Mary
Donnabelle Balela also wishes to thank the University of the Philippines
Engineering Research and Development Foundation, Inc. (UP ERDFI) for
the Robert Cheng/Uratex Professorial Chair in Engineering.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.scp.2020.100294.
Sustainable Chemistry and Pharmacy 17 (2020) 100294
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