Application of RSM for Bioremoval of Methylene Blue Dye from Industrial Wastewater onto Sustainable Walnut Shell (Juglans regia) Biomass
, Tatiana Minkina 2, Priyadarshani Rajput 2, Pinki Sharma 3, Anoop Kumar Verma 4, Smriti Agarwal 5 and Manoj Chandra Garg 1,*
Round 1
Reviewer 1 Report
Comments for author File: 
Comments.docx
Author Response
Q. In table no 2, the ligand represents the chemical composition of the walnut shell but in detail, it is considered hot water, and ethanol …. Are they really the composition of the walnut shell??? So kindly justify it!!!!
Response: Regarding extractives (10.2%), the highest amount belongs to water extractives 4.6%, followed by dichloromethane 2.9% and ethanol 2.7%. Please refer to reference no 22. We have corrected the word “hot water” to “water” in the table 2.
“Idalina, D.; José, F.; Bruno, E. Liquefaction and Chemical Composition of Walnut Shells. 2022
Q. In line no 108 you mentioned that you used 105 C for dry. Is it accepted? Because at this high temperature I think most of the walnut shells get burned.
Response: Authors are thankful to reviewer to point out this mistake. It is a typing error. Temperature used for walnut shells is 70oC. As suggested by reviewer, the authors have corrected the mistake (Please refer to line 131)
Q. In line no 186 you write the references as [26] [27,28] whereas in line no 189 you write [30–32], so kindly use the uniform pattern as per journal guidelines.
Response: Authors would like to thank the reviewer for highlighting this point. With regards to the mentioned point, the corrections have been made to the revised manuscript.
Q. The data of table no 5 is different as compared to the cited text from line no 207 to 210.
Response: With regard to these lines please refer to run 5 in table 4 (please refer line no. 239 to 241). Text regarding have been updated in line 267 and 270.
Q. In fig no 1 you should correct the axis label with “actual value” and “predicted value” instead of only “actual” and “predicted”. Same as in fig no 2 B.
Response: Correction has been made in revised manuscript. Please refer to Figure 1, lines no. 270 and Figure 2B 307.
Q. Section 2.6, line 166- “All variables were coded with five levels: 1, 0, +1, +, with = +2 functioning as the axial level”. Please see and justify “with = +2 functioning as the axial level”. Also have a look at line 182 in table 3, where α is repeated twice in range and levels.
Response: The authors appreciate the reviewer pointing out this error. The manuscript has been updated with the recommended suggestion (please refer to line no. 189-190 and 206).
Q. Table 4, lines 219 & 241. What does A, B, C, and D represent? It seems odd and should be mentioned in line 219 itself instead of line 241 (mentioned at bottom of the table, should be in the table heading along with dye removal %).
Response: The manuscript has been updated with the suggested correction (please refer line no. 248).
Q. Line 269: “Figure 1, illustrates that the predicted value of MB adsorption is plotted against the actual value from data, yielding the R2 value of 0.9334”. Where is this value in figure 1?
Response: On the manuscript, suggested corrections are made. Please refer to fig. 1 and line no. 285.
Q. WNS and MB stands for what? Should be mentioned at first instance. Moreover, at one place WS is used instead of WNS.
Response: Suggested correction is applied to the manuscript. WNS and MB stand for walnut shells and methylene blue.
Q. Kindly check sentence formation in entire MS as there are some sentence/word errors (e.g. line 307-317).
Response: The reviewer's attention to this point is appreciated, and the authors thank you. Corrected in manuscript.
Q. In references, journal name pattern is not uniform. e.g. 5,6,15,50 and so on. Please correct and give uniform pattern according to journal instructions
Response: Authors would like to thank the reviewer for highlighting this point. With regards to the mentioned point, the corrections have been made to the revised manuscript.
Reviewer 2 Report
· A number of studies are available on dye removal. Authors must highlight the novelty of the study conducted.
· Line 21-22: Authors must thoroughly check the manuscript and rectify all the grammatical errors like in the statement “To determine the independent variables, response surface methodology (RSM) is based on a face-centered central composite design is used”.
· There are a lot of errors in the statement formation. The use of present tense does not make sense for the experiments conducted in the past
· Paragraph 1 in the introduction section may be removed and a discussion of RSM must be elaborated in the introduction part.
· Line 181: References are missing for the independent parameters ranges, and levels used in the RSM model shown in table 3
· Authors should explain figures 3 and 4 in more detail that how different parameters are varying on different axes.
· Conclusion part is poorly written and needs revision. The introduction, Methodology, and results should not be repeated as such in the conclusion section of the manuscript.
Author Response
Q. A number of studies are available on dye removal. Authors must highlight the novelty of the study conducted
Response: Authors would like to thank the reviewer for the suggestion. With regards to the suggestion, the corrections have been made to the revised manuscript in line 107-115. The changes are shown below:
“According to prior study, the effects of plant-based biosorbent on various water quality dye wastewater are diverse. Therefore, it is necessary to determine how the coexistence of these variable parameters would affect the adsorption. However, more systematic data is still needed to fully comprehend the adsorption behaviour of cationic methylene blue dyes. Therefore, the two objectives of the current study were to:
- Use a locally available walnut shell as a precursor to creating nano biomass with high biosorption capacity and a cheap cost product.
- Using experimental design methodologies for optimization of selected parameters, explore the possible removal of biomass adsorption for methylene blue.”
Q. Line 21-22: Authors must thoroughly check the manuscript and rectify all the grammatical errors like in the statement “To determine the independent variables, response surface methodology (RSM) is based on a face-centred central composite design is used”.
Response: With regards to the suggestion, the corrections have been made to the revised manuscript in lines 21-22. The changes are shown below:
“Response surface methodology (RSM), is based on a face-centred central composite design, used to identify the independent variables.”
Q. There are a lot of errors in the statement formation. The use of present tense does not make sense for the experiments conducted in the past
Response: Authors would like to thank the reviewer for the suggestion. The authors have given a repeated reading to identify errors, which can be seen from the corrections applied in the manuscript with changes.
Q. Paragraph 1 in the introduction section may be removed and a discussion of RSM must be elaborated in the introduction part
Response: Suggested correction is applied to the manuscript (Please refer to line no. 57-65).
“RSM is essentially a combination of statistical and mathematical techniques that can be used for process optimization, constructing models that take parameter interactions into account, and conducting tests. The primary goal of RSM is to acquire the system's ideal operational conditions or an area that meets the operating requirements. RSM involves six sequential steps for the simulation and optimization of physicochemical processes (1) screening independent variables and selecting desired responses, (2) selecting an experimental design strategy, (3) conducting the experiments and obtaining the results, (4) fitting the mathematical model obtained to experimental data, (5) validating the model using graphs and analysis of variance, and (6) determining the optimal conditions.”
Reference
Behbahani, M., Alavi Moghaddam, M.R., Arami, M., 2011. Techno-economical evaluation of fluoride removal by electrocoagulation process: optimization through response surface methodology. Desalination 271:209–218. https:// doi.org/10.1016/j.desal.2010.12.033
Khedmati, M., Khodaii, A., Haghshenas, H.F., 2017. A study on moisture susceptibility of stone matrix warm mix asphalt. Constr. Build. Mater. 144:42–49. https://doi.org/ 10.1016/j.conbuildmat.2017.03.121
Q. Line 181: References are missing for the independent parameter’s ranges, and levels used in the RSM model shown in table 3
Response: A suggested change is made to the document. Please refer to line no. 212.
“Yadav, V., Ali, J., 2020. Biosorption of Methylene Blue Dye from Textile-Industry Wastewater onto Sugarcane Bagasse: Response Surface Modeling, Isotherms, Kinetic and Thermodynamic Modeling.”
Q. Authors should explain figures 3 and 4 in more detail that how different parameters are varying on different axes.
Response: Authors would like to thank the reviewer for the suggestion. With regards to the suggestion, the corrections have been made to the revised manuscript as shown in line 331-335, line 367-371, 388-391 and line 403-408. The changes are shown below:
“Fig. 3A–C shows how the effect of the biosorbent dose interacts with three other independent factors. It has been noted that as the amount of biosorbent is increased from 10 to 20 mg, dye removal increases at every range of temperature, pH, and concentration value (Fig. 3A, 3B and 3C, respectively).
Effect of initial dye concentration with 3 other independent variables have been illustrated in Fig 3C, 3D and 3F. As can be seen in Fig. 3C, at higher value of biosorbent dose, dye removal marginally rises when the initial dye concentration is increased from 20 to 40 mg/L, but it remains unaltered on lower value of biosorbent dose. Additionally, with increasing dye concentration, a modest increase in dye removal was seen at all pH and temperature values (Fig 3D and 3F).
Figs. 3B, 3D, and 3E show how the initial dye pH affects three other independent variables. According to Fig. 3B, dye removal increases as pH rises from 5 to 7 at lower range of biosorbent doses. However, pH had no impact on dye removal at lower biosorbent doses (Fig. 3B) or at every range of initial dye concentration (Fig. 3D). Additionally, it has been noted that dye removal was reduced when pH was raised at higher range temperatures value, but unaffected at lower range of temperature value (Fig 3E).
Effect of dye solution temperature with 3 other independent variables have been illustrated in Fig 3A, 3E and 3F. Dye removal was remaining unaffected with temperature as shown in Fig 3A and 3F. However, at higher value of pH slight decrease in dye removal was seen with increasing temperature from 20 to 30 oC (Fig 3E).”
Q. The conclusion part is poorly written and needs revision. The introduction, Methodology, and results should not be repeated as such in the conclusion section of the manuscript.
Response: The authors thank the reviewer for giving his/her comment. As suggested, conclusion part is revised. Please refer to line no. 486-508 as shown below:
“One large class of organic pollutants called dyes is recognized to have harmful effects on both people and aquatic habitats. Agriculture-based adsorbents have gained popularity in the textile sector, especially in the area of adsorption. In this work, walnut shell biomass was employed as a biosorbent to remove methylene blue dye from an aqueous solution. The biosorbent effectively eliminated the methylene blue from the solution. Methylene blue biosorption was investigated as a function of temperature, biomass dosage, initial pH and dye concentration. The ideal condition for maximal MB removal percentage was a biomass concentration of 18.24 gm, an initial pH level of 6.40, a dye concentration of 31.71 mg/l and a temperature of 21.7 oC. The experiments of MB were reduced by 97.74%. To maximize the effectiveness of the experiments, the face-centred central composite design matrix was successfully applied. The statistical model's actual and anticipated response values yielded satisfactory results that showed the elements under study had a positive impact on the biosorption of methylene blue by the walnut shell. The adsorbent removed a specific dye well, and its application to other dyes was possible. The current study investigates a sustainable approach to using potential waste biomass for dye industry wastewater treatment. Further advancement of the present biosorption phenomena serve as the foundation for a new technology intended to remove various pollutants from aqueous environments.
The authors would like to thank the reviewer for sparing their precious time in critically reviewing the manuscript. The respected reviewers’ technical comments and valuable productive suggestions will help in improving the quality of this manuscript according to the journal’s standards.
Reviewer 3 Report
The paper presented on methylene blue adsorption is very interesting and proposes a low-cost adsorbent, which is very significant.
It would be good to add adsorption desorption results for future studies as well as information on the final treatment of the biomass that now contains the contaminant.
Author Response
The paper presented on methylene blue adsorption is very interesting and proposes a low-cost adsorbent, which is very significant.
Response: The authors thank the reviewer for giving his/her comment.
Q. It would be good to add adsorption-desorption results for future studies as well as information on the final treatment of the biomass that now contains the contaminant.
Response: Authors would like to thank the reviewer for the suggestion. As a result of adsorption-desorption findings, the current paper will be rather lengthy, so we intend to undertake these investigations and publish the results in the following section.
Reviewer 4 Report
Ø Graphical Abstract should be included in the manuscript to invite wider readership
Ø In the aims and objectives of the study, authors have stated percentage of respective mechanism. It has to be specifically highlighted in the result and discussion section.
Ø Sampling location in fig. 1 should be identified to describe it properly.
Ø Study has stated three categories of removal efficiency but fails to highlight it in result and discussion section. The three categories defined should be incorporated in the result and discussion section.
Ø Add the purity, CAS numbers and company details of materials and chemicals
Ø Add the Tables for temperature pressure conditions. Also explain the details on methodology adopted
Ø Add the values of results in abstract, conclusion.
Ø Authors also can write about the impact of current work on the future research and industry
Ø Highlight the problem statement of the current work in the abstract and conclusion
Ø Check for grammatical errors and typos and improve the literature such as
https://doi.org/10.1016/j.chemosphere.2022.135738
https://doi.org/10.1016/j.envres.2022.114241
https://doi.org/10.1016/j.fuel.2021.122296
Author Response
Q. Graphical Abstract should be included in the manuscript to invite a wider readership
Response: Graphical Abstract is included in the manuscript before reference. (Line 522).
Q. In the aims and objectives of the study, the authors have stated the percentage of respective mechanisms. It must be specifically highlighted in the result and discussion section.
Response: As suggested, the aims and objectives have been highlighted in the result and discussion section, which can be read from lines 327-411.
Q. The study has stated three categories of removal efficiency but fails to highlight them in the result and discussion section. The three categories defined should be incorporated in the result and discussion section
Response: Authors would like to thank the reviewer for the suggestion. With regards to the suggestion, the corrections have been made to the revised manuscript line 331-335, line 367-371, 388-391 and line 403-408. The changes are shown below:
“Fig. 3A–C shows how the effect of the biosorbent dose interacts with three other independent factors. It has been noted that as the amount of biosorbent is increased from 10 to 20 mg, dye removal increases at every range of temperature, pH, and concentration value (Fig. 3A, 3B and 3C, respectively).
Effect of initial dye concentration with 3 other independent variables have been illustrated in Fig 3C, 3D and 3F. As can be seen in Fig. 3C, at higher value of biosorbent dose, dye removal marginally rises when the initial dye concentration is increased from 20 to 40 mg/L, but it remains unaltered on lower value of biosorbent dose. Additionally, with increasing dye concentration, a modest increase in dye removal was seen at all pH and temperature values (Fig 3D and 3F).
Figs. 3B, 3D, and 3E show how the initial dye pH affects three other independent variables. According to Fig. 3B, dye removal increases as pH rises from 5 to 7 at lower range of biosorbent doses. However, pH had no impact on dye removal at lower biosorbent doses (Fig. 3B) or at every range of initial dye concentration (Fig. 3D). Additionally, it has been noted that dye removal was reduced when pH was raised at higher range temperatures value, but unaffected at lower range of temperature value (Fig 3E).
Effect of dye solution temperature with 3 other independent variables have been illustrated in Fig 3A, 3E and 3F. Dye removal was remaining unaffected with temperature as shown in Fig 3A and 3F. However, at higher value of pH slight decrease in dye removal was seen with increasing temperature from 20 to 30 oC (Fig 3E).”
Q. Add the purity, CAS numbers and company details of materials and chemicals
Response: CAS number of methylene blue is 61-73-4 and was purchased from central drug house Pvt. Ltd. New Delhi and added in manuscript line no. 125-126 and Table 1.
Q. Add the Tables for temperature-pressure conditions. Also, explain the details of the methodology adopted
Response: Authors would like to thank the reviewer for the suggestion. The table for temperature conditions is already mentioned in column 5 in table 4 and the pressure condition is not used in this study.
Q. Add the values of results in the abstract, conclusion
Response: The values of results is added in the abstract and conclusion, as suggested by reviewer. (Line no. 26-28, 493 and 496)
Q. Authors also can write about the impact of current work on future research and industry
Response: Authors would like to thank the reviewer for the suggestion. With regards to the suggestion, the modification have been made to the revised manuscript in line no. 504-508:
“Current study investigates a sustainable approach to using potential waste biomass for dye industry wastewater treatment. Further advancement of the present biosorption phenomena serve as the foundation for a new technology intended to remove various pollutants or recover valuable resources from aqueous environments.”
Q. Highlight the problem statement of the current work in the abstract and conclusion
Response: Authors have added the problem statement in conclusion section (line no. 486-488), however it is already there in abstract section (line no. 17-19).
Q. Check for grammatical errors and typos and improve the literature such as
https://doi.org/10.1016/j.chemosphere.2022.135738
https://doi.org/10.1016/j.envres.2022.114241
https://doi.org/10.1016/j.fuel.2021.122296
Response: Authors would like to thank the reviewer for highlighting the errors and typos. With regards to the mentioned typo, the corrections have been made to the revised manuscript.
The authors would like to thank the reviewer for sparing their precious time in critically reviewing the manuscript. The respected reviewers’ technical comments and valuable productive suggestions will help in improving the quality of this manuscript according to the journal’s standards.
