Heavy Metals Distribution and Source Identification in Contaminated Agricultural Soils: Isotopic and Multi-Model Analysis
, Min Yang 1, Xinhong Gan 1, Lin Chen 1, Xiaohan Wang 1, Ming Li 1, Yuanyuan Lu 1 and Jian Xu 1,*Round 1
Reviewer 1 Report (Previous Reviewer 1)
Comments and Suggestions for AuthorsMy previous comments were successfully implemented to the manuscript. I have no further significant comments or remarks.
Author Response
Dear Reviewer,
How are you!
Thank you for your help in our manuscript and all the comments helped us greatly to revise and improve the paper.
Kind regards,
Jian Xu
Reviewer 2 Report (Previous Reviewer 2)
Comments and Suggestions for Authors# 1
In the existing literature, there are different approaches to determining the sources of Ni, Cu, and Cr concentrations from those you present. As the contribution rate of coal combustion, which you obtained according to the UNMIX model, is dominant (Chapts. 3.3.2 and 4), I suggest reading the results in the paper with DOI: 10.2428/ecea.2013.20(12)130 and discussing them in your Chapt. 3.
# 2
line 203: should be ‘hotspots’ instead of ‘hotpots’
Author Response
Dear Reviewer,
How are you!
Thank you for your help in our manuscript and all the comments helped us greatly to revise and improve the paper.
comment# 1[In the existing literature, there are different approaches to determining the sources of Ni, Cu, and Cr concentrations from those you present. As the contribution rate of coal combustion, which you obtained according to the UNMIX model, is dominant (Chapts. 3.3.2 and 4), I suggest reading the results in the paper with DOI: 10.2428/ecea.2013.20(12)130 and discussing them in your Chapt. 3.]
Response: Agreed and added this reference. The co-authors have thoroughly read this article and it was cited in this manuscript.
comment# 2[line 203: should be ‘hotspots’ instead of ‘hotpots’]
Response: Agreed and revised.
Sincerely yours
Jian Xu
Reviewer 3 Report (Previous Reviewer 3)
Comments and Suggestions for Authors1. As being a revised paper, I cannot see the improvements done, as the authors have not highlighted (in a different, visible colour) the corrections/completions in the newly revised manuscript. After I checked, nothing I suggest in my first reviewer report was not provided.
2. I do not understand why there is a Supplentary material, when all data in that material should be in the main text.
3. Please provide complete information regarding the apparatus and chemicals used in the experimental stage:
- the Model, Producer/manufacturer, City, and Country for EACH/ALL APPARATUS (4 information) used in the research, and
- the Producer, Country, purity degree, and concentration or CAS (4 information) for EACH REAGENT/chemical used in the research. Check the entire manuscript in this regard. This information gives the possibility for replicating you experiment to other authors and are requested in ALL journals.L393. Why cluster of 6 references, as 1 or 2 are enough to support a statement? Only for adding them?
6. What is the impact of anthropogenic aspects and climatic factors on long term soil monitoring and management related to heavy metal accumulation? https://doi.org/10.1007/s11356-021-14127-7
7. Future directions should be provided, maybe in a Figure format.
8. Last paragraph of Discussion must be added, describing the Strengths and the weakness/limitations of your research/results.
9. At the final of the manuscript, before references, complete Authors contribution section, according to the journal's draft. For correct detailing the Author Contributions section, you must follow the ethics in publications and the journal policies, better detailing these contributions. Check and respect the guide https://www.icmje.org/recommendations/browse/roles-and-responsibilities/defining-the-role-of-authors-and-contributors.html
10. References are numbered twice. Check and revise. Comments on the Quality of English LanguageGood English
Author Response
Dear Reviewer,
How are you!
Thank you for your help in our manuscript and all the comments helped us greatly to revise and improve the paper.
comment 1# As being a revised paper, I cannot see the improvements done, as the authors have not highlighted (in a different, visible colour) the corrections/completions in the newly revised manuscript. After I checked, nothing I suggest in my first reviewer report was not provided.
Response: Agreed and added. The revised manuscript with change marks was uploaded in submitting system and all the corrections were shown in revision mode.
comment 2# I do not understand why there is a Supplentary material, when all data in that material should be in the main text.
Response: There was a limitation in the body length, so the figures and tables which were auxiliary to explain the results of this research were listed in the Supplentary material.
comment 3# Please provide complete information regarding the apparatus and chemicals used in the experimental stage:the Model, Producer/manufacturer, City, and Country for EACH/ALL APPARATUS (4 information) used in the research, andthe Producer, Country, purity degree, and concentration or CAS (4 information) for EACH REAGENT/chemical used in the research. Check the entire manuscript in this regard. This information gives the possibility for replicating you experiment to other authors and are requested in ALL journals. L393. Why cluster of 6 references, as 1 or 2 are enough to support a statement? Only for adding them?
Response: Agreed and revised. The entire manuscript was checked and the Producer, Country, purity degree, and concentration used for each chemical used was added. The machine which determined the concentration of heavy metals and Hg species were also added with model, producer and country and the analytical method weas also referred on the original method. For the references of Hg isotope analysis, reference 58, 59 and 62 found the mass independent isotope fractionation (MIF, such as Δ199Hg or Δ200Hg) and mass dependent fractionation (MDF, such as δ202Hg). Besides, Hg isotope analysis can provide a practical pathway to verify source identification in soil pollution which can be referred in reference 60, 61 and 63. The order and method of references arranging was corrected.
comment 4# Statistical analysis. Soft used should be referenced.I suggesthttps://www.ibm.com/support/pages/how-cite-ibm-spss-statistics-or-earlier-versions-spss or similar links.
Response: Agreed and revised.
comment 5# How can you characterizethe toxicological impact of heavy metals on human health? I suggest checking and referring to https://doi.org/10.3390/toxics10120716
Response: Agreed and this paper was cited in the references. The paper named “Characterization of the Toxicological Impact of Heavy Metals on Human Health in Conjunction with Modern Analytical Methods” framed the already-published information on the topic, this review aimed to explore the toxicity of heavy metals to human health, the harmful effects of their accumulation, the advantages vs. the disadvantages of choosing different biological fluids/tissues/organs necessary for the quantitative measurement of heavy metals in the human body, as well as the choice of the optimal method, correlated with the purpose of the analysis. The paper found although heavy metal naturally in the environment, in volcanic eruptions or soil, but they are also the result of various human activities, such as mining, automobile emissions, and industrial waste, etc.
comment 6# What is the impact of anthropogenic aspects and climatic factors on long term soil monitoring and management related to heavy metal accumulation? https://doi.org/10.1007/s11356-021-14127-7
Response: Agreed this paper was cited in the references. This article is an extensive collection of scientific literature related to the impact of fertilizers on soil quality. It would be beneficial to follow clear directions, of which the following should be mentioned: rational use of fertilizers; the use of chemical compounds, as less harmful as possible for the health of those who consume agricultural products (humans and animals); more intensive use of natural fertilizers (i.e., manure from domestic animals) to the detriment of chemical, so that the health of the population does not suffer; clear indication, on the labels of agricultural products, of the substances that have been used for production to decrease the accumulation heavy metals.
comment 7# Future directions should be provided, maybe in a Figure format.
Response: Agreed and revised. Future directions were added in the Conclusion.
comment 8# Last paragraph of Discussion must be added, describing the Strengths and the weakness/limitations of your research/results.
Response: Agreed and revised. The strengths were described as follow: This study can accurately quantify and identify the factors contributing to heavy metal contamination in agricultural soil in a nano-scale. The sources of heavy metals were mainly enriched by the effects of the industrial activities especially coal combustion and traffic emissions.
comment 9# At the final of the manuscript, before references, complete Authors contribution section, according to the journal's draft. For correct detailing theAuthor Contributions section,you must follow the ethics in publications and the journal policies, better detailing these contributions. Check and respect the guide https://www.icmje.org/recommendations/browse/roles-and-responsibilities/defining-the-role-of-authors-and-contributors.html
Response: Agreed and revised. The Author Contributions was described as follow: Conceptualization, Tingting Mu and Jian Xu; Methodology, Tingting Mu, Xinhong Gan and Lin Chen; Software, Benyi Cao, Xinhong Gan, Lin Chen and Yuanyuan Lu; Formal analysis, Benyi Cao, Lin Chen, Xiaohan Wang and Yuanyuan Lu; Investigation, Tingting Mu, Benyi Cao, Xinhong Gan, Lin Chen, Xiaohan Wang, Ming Li and Jian Xu; Writing – original draft, Tingting Mu, Min Yang, Xinhong Gan, Lin Chen, Ming Li, Yuanyuan Lu and Jian Xu; Writing – review & editing, Tingting Mu, Xinhong Gan, Lin Chen and Jian Xu; Project administration, Jian Xu.
comment 10# References are numbered twice. Check and revise.
Response: Agreed and revised.
Sincerely yours,
Jian Xu
Reviewer 4 Report (New Reviewer)
Comments and Suggestions for AuthorsThis article has an adequate approach to the objectives, is well experimentally designed, is robust and its results are relevant: This investigation could offer a broader understanding of soil pollution sources and their respective contributions. This information can be beneficial to the management of specific strategies for soil remediation and sustainable land management in agricultural settings.
I recommend, before being accepted for publication, the following modifications:
1) The quality of Figure 2 is low. Please improve the resolution of said figure.
1) Section 4 Conclusions. Please delete "and Future perspectives"
3) Line 436, change "he" to "the".
Author Response
Dear Reviewer,
How are you!
Thank you for your help in our manuscript and all the comments helped us greatly to revise and improve the paper.
comment 1) The quality of Figure 2 is low. Please improve the resolution of said figure.
Response: All the figures in this manuscript would be uploaded in a single files with a high resolution to editor.
comment 2) Section 4 Conclusions. Please delete "and Future perspectives"
Response: Agreed and deleted.
comment 3) Line 436, change "he" to "the".
Response: Agreed and deleted.
Sincerely yours,
Jian Xu
This manuscript is a resubmission of an earlier submission. The following is a list of the peer review reports and author responses from that submission.
Round 1
Reviewer 1 Report
Comments and Suggestions for AuthorsThe topic of the manuscript is very interesting, but there are a many parts that are difficult for me to understand.
In whole manuscript authors refer to figure S1 (line 195) S2 (line 226),…. But in my version of manuscript i am unable to find these figures, so i am unable to do a proper review.
Figure 1: It is not obvious what is on x-axis (probably concentration in mg/kg).
In text is (line 138-139): „Between November 2020 and February 2021, a thorough collection of 38 soil samples 138 from a 0-20 cm depth was executed in the study area, as illustrated in Fig. 1. „ But y-axis of figure is in range 0-100. That to me is an inconsistency between the text and the figure.
Crucial is interpretation of table 1.
Authors write in the manuscript:“ An analysis of heavy metal concentrations (Ci) against the background values (Bi) of Zhejiang province revealed that the average concentrations of Pb, Cd, As, Zn, and Cu were lower than the background values. The average concentration of Ni was slightly higher than the background value, approximately 1.05 times greater, while the Hg concentration was significantly higher, about 20.8 times greater.“
From my point of view is it corect just for Hg and Cd. From table 1 is obvious that mean concentration of Pb is 43,5 mg/kg and background value is 32,5 mg/kg but in text is that the average concentration of Pb, Cd, As,Zn and Cu were lower than the background values. The situation is similar for other elements.
Due to the crucial misinterpretation mentioned above, I recommend to reject the manuscript in this form.
Reviewer 2 Report
Comments and Suggestions for AuthorsDear Authors,
Your manuscript in its current form has numerous deficiencies, errors and there are contradictions in your description of the results. The argument should be reconsidered and correctly presented taking into account the remarks and comments I have made below. Note that the suggestions are not ranked in order of relevance, but as shortcomings appear in the text.
# Preliminary note: the supplementary materials, Tables and Figures, have not been made available.
# Abstract: Unclear position on significance and sources of mercury in samples (“severe”, “high”, but “moderate” in the same paragraph)
# Introduction:
# v. 61 The decrease in content with depth is not convincing evidence of the natural (geogenic) origin of HM. On the contrary, the trend is the opposite (compare papers: Minerals 2020, 10, 1140. https://doi.org/10.3390/min10121140; ). The next statement (# v. 63) is correct but contradicts the previous one.
# Abreviations are confusing (PCA v PAC)
# Though the authors cite almost exclusively Chinese sources, yet I would recommend additional consideration of the results of B. Li and team (EMAS: https://doi.org/10.1007/s10661-016-5744-y).
# Fig. 1 contrary to what is described in the text (vv.138-139), it does not illustrate the metal contents in the 0-20 cm interval. In addition, the horizontal axes are not described: there are no units, and the ranges of values are different for each metal, making it difficult to track the relationships.
# Chapt. 2.3 and following parts
# Isotope research is described too briefly and thus the description sounds enigmatic (v. 162).
# There is no explanation of how the reference values for the analyzed metals were adopted (v. 180, Tab. 1, and further places). Are they regional average values for topsoils, or for bottomsoils, or for entire soil profiles, or perhaps the metal content of the immediate bedrock of the soils. It is known that the values of pollution and environmental risk indices will strongly depend on this strategy. In my experience, the last of these options adopted for calculations gives the most realistic results.
# Chapt. 3
# Again, we learn that Hg levels are "abnormally high" (v. 202) and then that they pose a "moderate risk" (v. 217).
# v. 252-255 Since the profiles do not show values in the 0-20 cm range, it is difficult to guess what HM enrichment trend the authors have in mind.
# Fig. 2 is non-communicative for the same reasons as Fig. 1.
# Fig. 4
where are the blue crosses mentioned in the legend?
# Chapt 3.2, and v. 312, and Chapt. 3.3, and vv. 327, 332, 437
In the literature to date there are different approaches to determining the sources of Ni, Cu, Cr concentrations from those presented by the authors.
# v. 322 authors provided no information on local “geological formations” so it is no possibility to verify their claim
# v. 353 This statement is correct but contradicts the misrepresentation in the Introduction (v. 61)
# Conclusions
The conclusions are formulated too vaguely and inaccurately in relation to the results described in the manuscript. Reading only this section, one gets the impression that the findings could have been made without conducting such a labor-intensive and expensive study.
# I urge you to address the earlier-mentioned papers (and listed below), which should help you rethink your approach to the results obtained:
https://doi.org/10.1007/s10661-016-5744-y
Comments on the Quality of English LanguageMinor editing of English language required
Reviewer 3 Report
Comments and Suggestions for AuthorsThe authors focused on Heavy metal pollution and source apportionment of peri-urban agricultural soils in south-eastern China. Please see my suggestions below:
Abstract is too long. Please see the Instructions for authors. https://www.mdpi.com/journal/agronomy/instructions
References must be added in brackets in the text and as numbers. Please see the Instructions for authors https://www.mdpi.com/journal/agronomy/instructions which are given to be followed and applied for ALL requirements. Please proceed consequently.
Introduction. Develop a paragraph regarding heavy metals effects in human body – I suggest checking and referring to https://doi.org/10.3390/toxics10120716
L130. A satellite image would be relevant.
2nd section; please provide:
- the Model, Producer/manufacturer, City, and Country (4 information) for EACH APPARATUS (4 information) used in the research, and
- the Producer, Country, purity degree, and concentration (4 information) used for each REAGENT/chemical used. Check the entire manuscript in this regard.
2.4. Statistical analysis. Soft used should be referenced. I suggest https://www.ibm.com/support/pages/how-cite-ibm-spss-statistics-or-earlier-versions-spss or similar links.
3rd section.
Discussion part is too poor, develop it better:
- How are the enzymatic indicators of the soil affected by heavy metal infestation/accumulation in the soil? Check https://www.researchgate.net/publication/320617256_Enzymatic_Indicators_of_Soil_Quality and https://doi.org/10.37358/RC.17.10.5864
- What is the impact of anthropogenic aspects and climatic factors on long term soil monitoring and management related to heavy metal accumulation? https://doi.org/10.1007/s11356-021-14127-7
- Future directions should be provided, maybe in a Figure format.
- Last paragraph of Discussion must be added, describing the Strengths and the weakness/limitations of your research/results.
Conclusions section must be also numbered (as 4).
Back Matter sections must be added after Conclusions and completed. Please see the Instructions for authors. https://www.mdpi.com/journal/agronomy/instructions
Editing tool must be used for checking English in the manuscript.
Comments on the Quality of English LanguageReadable English. Minor editing.
