The Impact of Berberine Pharmaceutical Wastewater on Aerobic Granules Formation: Change of Granules’ Size

Round 1

Reviewer 1 Report

Please find the attached file.

Comments for author File: Comments.docx

Author Response

Dear editor

We sincerely thank you and the reviewers. We fully appreciate the comments from the reviewers about our paper submitted to Processes. For addressing the questions, we have done further density functional theory calculations, data analyses and more precise expressions, including but not limited to further discussions of catalytic sites and reactive oxygen species, the interaction between PMS and SMZ with different configurations, the influence of inorganic ions.

All comments have been incorporated and each is replied or explained point by point, which also have been marked in the revised manuscript. Below, please find the comments in black, followed by our responses in blue for each comment.

1. Line 1-2; Title: Only granule’s size was focused?

Thanks. The manuscript describe the aerobic granules formation fed with non toxic substrates (acetate) and toxic substrates (berberine). The COD removal efficiency, the characteristics including MLSS, MLVSS, SVI, SOUR, average diameter, particle size and morphology of aerobic granules were compared. Here, granule’s size and size distribution was key characteristics to focus on.

2. Line 13: Please write the full form of CECET L&T

The full form of CECEP L&T is “China Energy Conservation and Environmental Protection Liuhe Tianrong Environmental Technology Co., Ltd.” However, the name in website is “CECEP L&T Environmental Technology Co., LTD”.

3. Line 19-20: I could not understand this sentence it seems to be meaning less? To better understand the impact of berberine pharmaceutical wastewater treatment on the granule growth during aerobic granules formation, the particle size, size distribution of aerobic granules were traced over 81 days in three sequencing batch reactors fed with acetate and berberine wastewater.
4. Line 20. If I am not wrong, you can put and in between The particle size and size distribution? The particle size, size distribution.

Thank you for suggestion. The sentence revised to be “To better understand the impact of toxic compounds on aerobic granules’ growth during their formation, the particle size and size distribution of aerobic granules were traced over 81 days in three sequencing batch reactors fed with acetate and berberine wastewater.”  

 

5. In title you mentioned Berberine? Line 22. Acetate and berberine wastewater?

Thank you! In this manuscript, berberine represented toxic substrate and the target compound. While acetate represented the non-toxic substrate, the reference compound. Thus I mention berberine in title.

 

6. Abstract: Please add problem statement in first part. Here I am suggesting: problem statement in first part, Experimental work in second part and your results. I could not find the problems please add.

Thank you for your suggestion. The problem statement has been added in Abstract (P1).

7. It seems you did not fallow MDPI process guide lines. In next round please format your paper according to guide lines.

Thanks. The format has been revised according to guide lines.

 

8. Figure 1. Please enlarge the font size.

Thank you! The font sizes of Figure 1-figure 5 have been revised

 

9. Figure 1. I saw high influent concentration (greater than 1500mg/L). Did you observe inhibition?

Thank you! R1 was feed with acetate synthetic wastewater. R2 was feed with synthetic wastewater with the components of acetate and berberine. And the effluent from a anaerobic baffled reactor (ABR) which fed with industrial berberine wastewater was pumped into R3 as influent. Although the influent concentrations of three reactors was greater than 1500mg/L, there were almost no inhibition during the operation processes. Since berberine fed to R2 was mixed with acetate to reduce the inhibition effect and for R3, the inoculum was collected from the industrial wastewater treatment plant which influent contained berberine.

10. 1. process in R1, R2 and R3

Thanks. The word “process” has been changed to be “processes”.

 

11. Figure 4. Please fix the similar word formatting in all figures.

Thank you! The similar word formatting in all figures has been revised.

 

12. Please fix your format according to guidelines

Thank you! The format has been revised

 

Author Response File: Author Response.docx

Reviewer 2 Report

The paper is interesting.
I recommend publication only if the following issues can be addressed.

- Abstract: Include more of your results.

- The authors should report general information about Pharmaceutical Wastewater in the Introduction section.

- Lines 61-62 page 4: You should mention that discharge of BBR degrades water quality and thus it can not be directly used for potable water (via desalination) and industrial applications. Cite the following references:

Panagopoulos, A. (2020). A comparative study on minimum and actual energy consumption for the treatment of desalination brine. Energy, 212. 

Panagopoulos, A. (2021). Energetic, economic and environmental assessment of zero liquid discharge (ZLD) brackish water and seawater desalination systems. Energy Conversion and Management, 235.

Panagopoulos, A. (2021). Study and evaluation of the characteristics of saline wastewater (brine) produced by desalination and industrial plants. Environmental Science and Pollution Research, 1-14.

- How many replications you performed for your experiments?

- Conclusion: Include more of your results.

- Conclusion: Discuss the applicability of your findings/results and future study in this field.

- Language editing is recommended.

Author Response

Dear editor

We sincerely thank you and the reviewers. We fully appreciate the comments from the reviewers about our paper submitted to Processes. For addressing the questions, we have done further density functional theory calculations, data analyses and more precise expressions, including but not limited to further discussions of catalytic sites and reactive oxygen species, the interaction between PMS and SMZ with different configurations, the influence of inorganic ions.

All comments have been incorporated and each is replied or explained point by point, which also have been marked in the revised manuscript. Below, please find the comments in black, followed by our responses in blue for each comment.

1. Line 1-2; Title: Only granule’s size was focused?

Thanks. The manuscript describe the aerobic granules formation fed with non toxic substrates (acetate) and toxic substrates (berberine). The COD removal efficiency, the characteristics including MLSS, MLVSS, SVI, SOUR, average diameter, particle size and morphology of aerobic granules were compared. Here, granule’s size and size distribution was key characteristics to focus on.

2. Line 13: Please write the full form of CECET L&T

The full form of CECEP L&T is “China Energy Conservation and Environmental Protection Liuhe Tianrong Environmental Technology Co., Ltd.” However, the name in website is “CECEP L&T Environmental Technology Co., LTD”.

3. Line 19-20: I could not understand this sentence it seems to be meaning less? To better understand the impact of berberine pharmaceutical wastewater treatment on the granule growth during aerobic granules formation, the particle size, size distribution of aerobic granules were traced over 81 days in three sequencing batch reactors fed with acetate and berberine wastewater.
4. Line 20. If I am not wrong, you can put and in between The particle size and size distribution? The particle size, size distribution.

Thank you for suggestion. The sentence revised to be “To better understand the impact of toxic compounds on aerobic granules’ growth during their formation, the particle size and size distribution of aerobic granules were traced over 81 days in three sequencing batch reactors fed with acetate and berberine wastewater.”  

 

5. In title you mentioned Berberine? Line 22. Acetate and berberine wastewater?

Thank you! In this manuscript, berberine represented toxic substrate and the target compound. While acetate represented the non-toxic substrate, the reference compound. Thus I mention berberine in title.

 

6. Abstract: Please add problem statement in first part. Here I am suggesting: problem statement in first part, Experimental work in second part and your results. I could not find the problems please add.

Thank you for your suggestion. The problem statement has been added in Abstract (P1).

7. It seems you did not fallow MDPI process guide lines. In next round please format your paper according to guide lines.

Thanks. The format has been revised according to guide lines.

 

8. Figure 1. Please enlarge the font size.

Thank you! The font sizes of Figure 1-figure 5 have been revised

 

9. Figure 1. I saw high influent concentration (greater than 1500mg/L). Did you observe inhibition?

Thank you! R1 was feed with acetate synthetic wastewater. R2 was feed with synthetic wastewater with the components of acetate and berberine. And the effluent from a anaerobic baffled reactor (ABR) which fed with industrial berberine wastewater was pumped into R3 as influent. Although the influent concentrations of three reactors was greater than 1500mg/L, there were almost no inhibition during the operation processes. Since berberine fed to R2 was mixed with acetate to reduce the inhibition effect and for R3, the inoculum was collected from the industrial wastewater treatment plant which influent contained berberine.

10. 1. process in R1, R2 and R3

Thanks. The word “process” has been changed to be “processes”.

 

11. Figure 4. Please fix the similar word formatting in all figures.

Thank you! The similar word formatting in all figures has been revised.

 

12. Please fix your format according to guidelines

Thank you! The format has been revised

 

 

 

Reviewer 3 Report

You need to do the followings, to really improve your paper:

• ask a proficient technical English person to proofread your paper
• the introduction need to be rewritten, showing the state-of-the-art in the domain of your research
• you need to clearly show which are the novelties of your approach, apart from biologically removing berberine wastewater
• instead of describing the figures in the text, you need to explain the results presented in them
• when you use "esoteric" indexes, like D[4,3] or d(0.5), you must give their definitions and the respective formulas to compute them
• the experimental results must be, always, presented as "average +- standard deviation"
• the conclusions should summarize the original contributions

Author Response

Dear editor

We sincerely thank you and the reviewers. We fully appreciate the comments from the reviewers about our paper submitted to Processes. For addressing the questions, we have done further density functional theory calculations, data analyses and more precise expressions, including but not limited to further discussions of catalytic sites and reactive oxygen species, the interaction between PMS and SMZ with different configurations, the influence of inorganic ions.

All comments have been incorporated and each is replied or explained point by point, which also have been marked in the revised manuscript. Below, please find the comments in black, followed by our responses in blue for each comment.

1. Line 1-2; Title: Only granule’s size was focused?

Thanks. The manuscript describe the aerobic granules formation fed with non toxic substrates (acetate) and toxic substrates (berberine). The COD removal efficiency, the characteristics including MLSS, MLVSS, SVI, SOUR, average diameter, particle size and morphology of aerobic granules were compared. Here, granule’s size and size distribution was key characteristics to focus on.

2. Line 13: Please write the full form of CECET L&T

The full form of CECEP L&T is “China Energy Conservation and Environmental Protection Liuhe Tianrong Environmental Technology Co., Ltd.” However, the name in website is “CECEP L&T Environmental Technology Co., LTD”.

3. Line 19-20: I could not understand this sentence it seems to be meaning less? To better understand the impact of berberine pharmaceutical wastewater treatment on the granule growth during aerobic granules formation, the particle size, size distribution of aerobic granules were traced over 81 days in three sequencing batch reactors fed with acetate and berberine wastewater.
4. Line 20. If I am not wrong, you can put and in between The particle size and size distribution? The particle size, size distribution.

Thank you for suggestion. The sentence revised to be “To better understand the impact of toxic compounds on aerobic granules’ growth during their formation, the particle size and size distribution of aerobic granules were traced over 81 days in three sequencing batch reactors fed with acetate and berberine wastewater.”  

 

5. In title you mentioned Berberine? Line 22. Acetate and berberine wastewater?

Thank you! In this manuscript, berberine represented toxic substrate and the target compound. While acetate represented the non-toxic substrate, the reference compound. Thus I mention berberine in title.

 

6. Abstract: Please add problem statement in first part. Here I am suggesting: problem statement in first part, Experimental work in second part and your results. I could not find the problems please add.

Thank you for your suggestion. The problem statement has been added in Abstract (P1).

7. It seems you did not fallow MDPI process guide lines. In next round please format your paper according to guide lines.

Thanks. The format has been revised according to guide lines.

 

8. Figure 1. Please enlarge the font size.

Thank you! The font sizes of Figure 1-figure 5 have been revised

 

9. Figure 1. I saw high influent concentration (greater than 1500mg/L). Did you observe inhibition?

Thank you! R1 was feed with acetate synthetic wastewater. R2 was feed with synthetic wastewater with the components of acetate and berberine. And the effluent from a anaerobic baffled reactor (ABR) which fed with industrial berberine wastewater was pumped into R3 as influent. Although the influent concentrations of three reactors was greater than 1500mg/L, there were almost no inhibition during the operation processes. Since berberine fed to R2 was mixed with acetate to reduce the inhibition effect and for R3, the inoculum was collected from the industrial wastewater treatment plant which influent contained berberine.

10. 1. process in R1, R2 and R3

Thanks. The word “process” has been changed to be “processes”.

 

11. Figure 4. Please fix the similar word formatting in all figures.

Thank you! The similar word formatting in all figures has been revised.

 

12. Please fix your format according to guidelines

Thank you! The format has been revised

 

 

 

Round 2

Reviewer 1 Report

Dear authors, Thanks for reply of comments. Here are few comments you need to incorporate 1. Line 84. The SOUR was measured in (Experimental Investigation of substrate shock and Environmental ammonium concentration on the stability of ammonium-oxidizing bacteria (AOB). detailed description of SOUR, MLSS, and others parameters are available in above paper. 2. Figure 1. Looks fine but font size does not match with manuscript body. please correct.

Author Response

1. Dear editor

   We sincerely thank you and the reviewers. We fully appreciate the comments from the reviewers about our paper submitted to Processes.

   All comments have been replied to or explained point by point, which also has been marked in the revised manuscript. Below, please find the comments in black, followed by our responses in blue for each comment.

    

   Reviewer 1

   1. Line 84. The SOUR was measured in (Experimental Investigation of substrate shock and Environmental ammonium concentration on the stability of ammonium-oxidizing bacteria (AOB). detailed description of SOUR, MLSS, and others parameters are available in above paper.

   Response 1: Thank you. The paper has been cited as 24.

   2. Figure 1. Looks fine but font size does not match with manuscript body. please correct.

   Response 2: Thank you for your suggestion. Figure1 has been revised.

    

Author Response File: Author Response.docx

Reviewer 2 Report

The paper is interesting.
I recommend publication only if the following issues can be addressed.

- Abstract: Include more of your results.

- The authors should report general information about Pharmaceutical Wastewater in the Introduction section.

- Lines 61-62 page 4: You should mention that discharge of BBR degrades water quality and thus it can not be directly used for potable water (via desalination) and industrial applications. Cite the following references:

Panagopoulos, A. (2020). A comparative study on minimum and actual energy consumption for the treatment of desalination brine. Energy, 212. 

Panagopoulos, A. (2021). Water-energy nexus: desalination technologies and renewable energy sources. Environmental Science and Pollution Research. 

Panagopoulos, A. (2021). Study and evaluation of the characteristics of saline wastewater (brine) produced by desalination and industrial plants. Environmental Science and Pollution Research, 1-14.

- How many replications you performed for your experiments?

- Conclusion: Include more of your results.

- Conclusion: Discuss the applicability of your findings/results and future study in this field.

- Language editing is recommended.

Author Response

Dear editor

We sincerely thank you and the reviewers. We fully appreciate the comments from the reviewers about our paper submitted to Processes.

All comments have been replied to or explained point by point, which also has been marked in the revised manuscript. Below, please find the comments in black, followed by our responses in blue for each comment.

Reviewer 2

1. Abstract: Include more of your results.

Response 1: The abstract has been revised.

2. The authors should report general information about Pharmaceutical Wastewater in the Introduction section.

Response 2: Thank you! The properties of berberine have been added in paragraph 2, P2. The detailed information on berberine pharmaceutical wastewater has been provided in 2.3. Medium (paragraph 5, P2).

 

3. Lines 61-62 page 4: You should mention that discharge of BBR degrades water quality and thus it can not be directly used for potable water (via desalination) and industrial applications. Cite the following references:

Panagopoulos, A. (2020). A comparative study on minimum and actual energy consumption for the treatment of desalination brine. Energy, 212.

Panagopoulos, A. (2021). Water-energy nexus: desalination technologies and renewable energy sources. Environmental Science and Pollution Research. 

Panagopoulos, A. (2021). Study and evaluation of the characteristics of saline wastewater (brine) produced by desalination and industrial plants. Environmental Science and Pollution Research, 1-14.

Response 3: Thank you for your suggestion! There is no point related to desalination and potable water in this manuscript. The recommended references will be cited in the next manuscript.

4. How many replications you performed for your experiments?

Response 4: Thank you. For the physical/chemical experiments, they can be repeated three times. For the batch scale wastewater treatment experiment, generally, they are repeated three times. For the continuously operated reactor, we collect every sample three times and tested them three times.

5. Conclusion: Include more of your results.

Response 5: Thank you! The conclusion has been revised.

 

6. Conclusion: Discuss the applicability of your findings/results and future study in this field.

Response 6: Thank you! The conclusion has been revised.

7. Language editing is recommended.

Response 7: Thank you! The language has been revised.

Author Response File: Author Response.docx

Reviewer 3 Report

The observations/comments are in the attached file.

Comments for author File: Comments.pdf

Author Response

Dear editor

We sincerely thank you and the reviewers. We fully appreciate the comments from the reviewers about our paper submitted to Processes.

All comments have been replied to or explained point by point, which also has been marked in the revised manuscript. Below, please find the comments in black, followed by our responses in blue for each comment.

 

Reviewer 3

1. You must report all the experimental values as "average +- standard deviation" throughout this paper

Response 1: Thank you! The experimented values have been reported as "average +- standard deviation".

2. You must remove this paragraph

Response 2: Thank you for your suggestion. The paragraph has been deleted.

 

3. You must explain:

- why there is a great discrepancy between what you declare here and the real influent COD concentrations presented in Fig. 1

- taking into account what you declared in section "2.3. Medium ", you must explain why the influent profiles of R2 and R3 are the same

- also, you must explain why the removal efficiency profiles of R2 and R3 are the same, although they have completely different influents -synthetic and from ABR.

Response 3: Thank you! The data have been checked, Fig.1 and the first paragraph of 3.1 have been revised. (3.1 Biological treatment performance during aerobic granulation in R1, R2, R3 of P3)

4. You need to rephrase the paragraph between lines 105 and 115; really difficult to understand, due to the way the information is delivered.

Also, you must explain the results reported in Fig. 2.

Response 4: Thank you! The paragraph between lines 105 and 115, including the explanation in Fig. 2 has been revised.

 

5. You must explain what is the meaning of this notation, never explained.

Response 5: Thank you! VSS means volatile suspended solids. SOUR means specific oxygen utilization rates. Both the two notations have been explained in L58, L59, P2.

 

6. You must explain what MLSS and MLVSS are and how these and SOUR represent characteristics of aerobic granules.

Response 6: Thank you! MLSS means mixed liquor suspended solids, and MLVSS means mixed liquor volatile suspended solids. Please find the revised explanation in L105-107, P3.

For accurate expression, the caption of Fig 2 has been revised as “Fig 2 The variations of MLSS, MLVSS, settleability (SVI), and microbial activity (SOUR) during aerobic granules’ formation process in R1, R2, andR3.”

7. You must give the relationships used to compute D[4,3] and d(0.5).Also, you must give, as an example, the density distribution of the diameters, say, for the day when d(05) is highest. And, always, report the experimental data as "average +- standard deviation"

Response 7: Thank you! D[4,3] and d(0.5) were provided by Mastersizer 2000. Here is the result of one sample. The calculation was finished by the software. The D[4,3] and d(0.5) were exported based on granularity data.

Consistency

Diameter distance

8. A much better index is the ration between the standard deviation and average (mean) - the smaller the value, the narrower the distribution. What are the measuring units of "diameter distance"? You must provide the computation relationship.

Response 8: Thank you! diameter distance = , which was explained in reference 31. d(0.9), d(0.1) and d(0.5) were provided by granularity analysis report by Mastersizer 2000.

31. Shu X.; Wu Y.C.; Tao Q.X.; Cheng J. G., Xia Y.H. An analysis on report of Mastersizer 2000 laser particle size analyzer. Experimental Technology.Management, 28, 37-41.
32. It is wrong to compare the reactors performance for different days. A better way is to report this value for the days 4, 50 and 81.

Response 9: Thank you! The comparison has been performed based on the same days’ data after revision. For example, the average value for a steady state is the average value from day 51 to day 74.

10. You must provide the computation formula. Also, you must explain why the granules from R3, which started with a higher consistence that those from R2, ended with a lower value. Also, why reporting from day 57, and not from day 4, in a table, five values, for five days equally spaced between days 4 and 81.

Response 10: Thank you! The consistency was provided by a granular analysis report from Mastersizer 2000. The comparison has been performed based on the same days’ data after revision. The changes in consistency in the three reactors have been revised (The fourth paragraph of 3.2).

11. In what is this different than 3.2? You must combine them, and discuss these distributions appropriately.

Response 11: Thank you! The title of 3.2 “Effects of berberine wastewater on the formation of aerobic granules” has been revised to be “Effects of berberine wastewater on the morphology of aerobic granules”. In 3.2, the average value of diameters was reported, just like most researchers have done. In 3.3, I’d like the auditor to zoom in, to see details of the granularity variety during the granulation process. In the published paper, the researcher made the same measurement using Mastersizer 2000, most of them just use D(4,3) as an indicator of the average diameter. I find more information if we make a detailed analysis of the size distribution.

12. Here, a lot of information already presented is duplicated.

Response 12: Thank you! The paragraph has been revised.

 

Author Response File: Author Response.docx