Reinforcement and Antibacterial Properties of Hand Embroidery Threads Based on Green Nanocoatings

Round 1

Reviewer 1 Report

1. Introduction section must be two paragraphs. The first one is related to the background of the study and the second one must be with the article. The first paragraph must mention a few articles' findings such as [https://0-doi-org.brum.beds.ac.uk/10.1016/j.enmm.2021.100485; https://0-doi-org.brum.beds.ac.uk/10.1002/slct.202003033] for the rational approach to this study. 

2. In the discussion section, the authors should mention the chemical interactions involved in the attachment of NPs with cotton thread with the help of some reference articles.

3. The article must mention some of the major metabolites present in the Molokhia stems, which are majorly responsible for the reduction and capping of NPs. Along with this, Authors could refer to the following book for this purpose as well (Terpenoids Against Human Diseases; March 21, 2019, by CRC Press)

4. Authors have described the results section well.

Author Response

Responses to the Comments of Reviewer #1

 

Reviewer #1: 1. Introduction section must be two paragraphs.

We thank the reviewer for imparting his valuable time in reviewing the manuscript and

acknowledging the importance of the research work and his useful comments and recommendation for publication.

1. Introduction section must be two paragraphs. The first one is related to the background of the study and the second one must be with the article. The first paragraph must mention a few articles' findings such as [https://0-doi-org.brum.beds.ac.uk/10.1016/j.enmm.2021.100485; https://0-doi-org.brum.beds.ac.uk/10.1002/slct.202003033] for the rational approach to this study.

(Authors’ Response) Thank you for reviewer comment. This is considered in revised version and the first and second paragraph was improved. Additionally, the suggested reports by reviewers were studied and cited in revised version and highlighted.

Inserted References

[5] Pal, A.; Goswami, R.; Roy, D. N. A critical assessment on biochemical and molecular mechanisms of toxicity developed by emerging nanomaterials on important microbes. Environ. Nanotech. Monit. Manage. 2021,16,100485

 

[6] Majumdar, M.; Khan, S. A.; Nandi N. B.;  Roy, S.; Panja, A. S.;  Roy, D. N.; Misra, T. K. Green synthesis of iron nanoparticles for investigation of biofilm inhibition property. Chemistryselect 2020, 5, 13575-13583.  

 

 

 

 

2. In the discussion section, the authors should mention the chemical interactions involved in the attachment of NPs with cotton thread with the help of some reference articles.

(Authors’ Response) Thank you for reviewer comment. This is considered in revised version and thus new section explaining the interaction between cotton surface and coating based ZnONPs layer. Thus, the following section and new references were inserted and highlighted as listed.

 

Inserted Section

(Pages 5-6) It is noteworthy to note that, the coating layer composed from MSE-ZnONP-ST was interacted to  the cotton hand embroidery threads surfaces via supramolecular interaction (H-Boding). Thus, the rich hydroxyl groups exist on the structure of MSE and ST capped and wrapped the ZnONPs form dense hydrogen bonding with hydroxy groups of cotton hand embroidery threads [27-28]. Therefore, these strengthen the interaction of the coating layer based on ZnONPs with cotton threads. 

 

Inserted references  

[27] Attia, N. F.; Moussa, M.; Sheta, A. M. F.; Taha, R.; Gamal, H.  Effect of different nanoparticles based coating on the performance of textile properties. Prog. Org. Coat. 2017, 104, 72-80.

 

[28] Poon, C. K.;  Kan, C. K.  Effects of TiO₂ and curing temperatures on flame retardant finishing of cotton. Carbohyd. Polym. 2017, 121, 457-467.

 

 

 

3. The article must mention some of the major metabolites present in the Molokhia stems, which are majorly responsible for the reduction and capping of NPs. Along with this, Authors could refer to the following book for this purpose as well (Terpenoids Against Human Diseases; March 21, 2019, by CRC Press)

(Authors’ Response) Thank you for reviewer comment. This is considered in revised version and thus new section explaining the major metabolites present in the Molokhia stems, which are majorly responsible for the reduction and capping of NPs. Thus, new section with new references were inserted and highlighted. Additionally, the suggested reference by reviewer was also cited.

 

Inserted Section

(Pages 2-3) Additionally, molokhia (Corchorus olitorius L.),  a well-known Egyptian vegetable also known as Egyptian spinach, is also grown in large quantities every year. Unexpectedly, it was discovered that molokhia extract has a wealth of beneficial phenolic and antioxidant chemicals such as such as vitamin C, vitamin E, β-carotene, α-tocopherol, glutathione, and phenols  [16-18] that have the potential to function as potential reducing agents to metal ions [19]. This is in addition of exitance of terpenoids which serve as capping for prepared metal nanoparticles [ 20-21].

Inserted references

[17] Simopoulos, A. P.; Norman, H. A.; Gillaspy,  J. E. Purslane in human nutrition and its potential for world agriculture. World Rev. Nutr. Diet. 1995,77, 47-74.

[18] Azuma, K.; Nakayama, M.; Koshioka, M.; Ippoushi, K.; Yamaguchi, Y.; Kohata, K.; Yamauchi, Y.; Ito, H.; Higashio, H. Phenolic Antioxidants from the Leaves of Corchorus olitorius L. J. Agric. Food Chem. 1999, 47, 3963-3966.

[19] Ismail, E. H.; Saqer, A. M. A.; Assirey, E.; Arshi Naqvi, A.; Okasha, R. M. Successful green synthesis of gold nanoparticles using a corchorus olitorius extract and their antiproliferative effect in cancer cells. Int. J. Mol. Sci. 2018, 19, 2612.

[20] Haque, M. J.; Bellah, M. M.; Hassan, M. R.; Rahman, S. Synthesis of ZnO nanoparticles by two different methods comparison of their structural, antibacterial, photocatalytic and optical properties. Nano Express 2020, 1, 010007.

[21] Nath Roy, D. Terpenoids Against Human Diseases. CRC Press, Boca Raton, 2019.

4. Authors have described the results section well.

(Authors’ Response) Thank you for reviewer comment and his positive recommendation.

Author Response File: Author Response.doc

Reviewer 2 Report

In this paper, a novel green nanocoating for hand embroidery thread was designed and fabricated. Uniform, narrow particle size dispersible ZnONPs were synthesized from Konjac stem extract, which could be coated on hand embroidery thread after being wrapped with starch chains. The new green nano-coating can effectively improve the tensile strength of hand embroidery thread, and inhibit the growth of bacteria on hand embroidery thread. I think this paper can be revised and published in this journal. The suggestions are as follows.

1.The content of the article is messy and poorly organized, so it needs to be adjusted and modified.

2.The picture in the text contains less information, so you can annotate some content in the picture.

3.The picture in Figure 2 has less information and should be marked clearly. And is it necessary to enlarge b and c by two different multiples?

4.How to calculate the size of the transparent inhibition zone, and whether the placement of the hand embroidery line will cause an impact.

5.The data in the text are mostly tabulated, which can be expressed more clearly by a line chart or bar chart.

Author Response

Responses to the Comments of Reviewer #2

Reviewer # 2. In this paper, a novel green nanocoating for hand embroidery thread was designed and fabricated. Uniform, narrow particle size dispersible ZnONPs were synthesized from Konjac stem extract, which could be coated on hand embroidery thread after being wrapped with starch chains. The new green nano-coating can effectively improve the tensile strength of hand embroidery thread, and inhibit the growth of bacteria on hand embroidery thread. I think this paper can be revised and published in this journal. The suggestions are as follows.

1.The content of the article is messy and poorly organized, so it needs to be adjusted and

modified.

(Authors’ Response) Thank you for reviewer comment. This is considered in revised version and the manuscript was strongly organized and modified in revised version and highlighted.

2. The picture in the text contains less information, so you can annotate some content in

the picture.

(Authors’ Response) Thank you for reviewer comment. This is considered in revised version and all pictures were modified in revised version and highlighted.

 

3.The picture in Figure 2 has less information and should be marked clearly. And is it

necessary to enlarge b and c by two different multiples?

 

(Authors’ Response) Thank you for reviewer comment. This is considered in revised version Figure 2 was modified and image was replaced and the dispersion of ZnONPs were highlighted in Images. Hence, Figure was modified in revised version as listed.

4.How to calculate the size of the transparent inhibition zone, and whether the placement of the hand embroidery line will cause an impact

(Authors’ Response) Thank you for reviewer comment. Actually, the antibacterial activity of samples against staphylococcus aureus bacteria was investigated using the AATCC standard test method 147-2004 [31]. The average clear inhibition zone W in mm was evaluated based on this equation W = (T-D)/2 where T is the total diameter of both test specimen and clear zone in mm and D is width of the test specimen only in mm. Thus, in experimental section this section was inserted and revised.

Actually, the placement hand embroidery line has no influence on the clear inhibition zone.

Inserted Section

(Page 4) Using the AATCC standard test method 147-2004 [23], the antibacterial activity of samples against Staphylococcus aureus bacteria was examined. Based on this equation, W = (T-D)/2, where T is the entire diameter of the test specimen and clear zone in mm and D is the test specimen's width only in mm, then, the average clear inhibition zone W in mm was calculated.

 

Inserted Reference

[23] AATCC Test Method 147, Antibacterial activity assessment of textile materials parallel streak methods: parallel streak method (2004)

 

5.The data in the text are mostly tabulated, which can be expressed more clearly by a line chart or bar chart.

 

(Authors’ Response) Thank you for reviewer comment. This is considered in revised version and tensile strength data were depicted in Figure 5.

 

Inserted Figure

Author Response File: Author Response.doc

Reviewer 3 Report

Alshehri et al. presented a method to utilize molokhia stem extract as the reducing agent to prepare narrowly-dispersed ZnO NP for rendering hand embroidery thread with higher mechanical strength and antibacterial property. Some problems in this manuscript still have to be addressed before it can be recommended for publication.

 

1.    Molokhia stems extract (MSE) as a mixture was used as reducing agent for zinc acetate in this research, the authors should provide more information of which detailed chemical inside MSE is offering this reducing property and the concentration of this agent in the MSE.

2.    More detailed synthetical mechanism of the ZnO NP should be provided, including the role of elevating pH value, why use zinc acetate as the precursor for the sol-gel process, and the role of oxygen in the ZnO formation process.

 

3.    How does starch help the ZnO NP to deposit onto hand embroidery thread? More explanation on the depositing process should be provided. Also, the MSE-ZnONP-ST is supposed to have a “core-shell” structure, but no such feature can be observed in Figure 2. The authors are encouraged to provide better TEM images and measure the shell size of the starch coating layer.

 

4.    For Figure 4 SEM-EDS mapping images, it seemed like the elements were just randomly scattered over the observatory field. The authors may consider to overlay the mapping images over the original SEM secondary electron image to better assign each element spot to an exact structure of your specimen.

 

 

5.    In Tensile test section, the authors summarized the tensile strength in a unit of N, since all the hand embroidery threads have different width, we may consider calculating the tensile strength in a unit of kPa for a better presentation and comparison of the results.

6.    For antibacterial test, the authors should also test the performance on Gram-negative bacteria like E. coli, only one type of bacteria test does not formulate a compelling result. Also, in Figure 5, there were too much variance in the size of the threads loaded for the inhibitory zone test. The authors should use the same weight of thread for each sample and fold them into the same size then load onto culture plate.

7.    Section 2.3 should be titled as “Preparation of coated hand embroidery threads” instead of “Synthesis of hand embroidery threads coatings”.

8.    There are two “and” neighboring to each other in Page 2 line 87, please delete one of them.

Author Response

Responses to the Comments of Reviewer #3

 

Reviewer # 3 Alshehri et al. presented a method to utilize molokhia stem extract as the reducing agent to prepare narrowly-dispersed ZnO NP for rendering hand embroidery thread with higher mechanical strength and antibacterial property. Some problems in this manuscript still have to be addressed before it can be recommended for publication.

 We thank the reviewer for imparting his valuable time in reviewing the manuscript and

acknowledging the importance of the research work and his useful comments and recommendation for publication.

 

1. Molokhia stems extract (MSE) as a mixture was used as reducing agent for zinc acetate in this research, the authors should provide more information of which detailed chemical inside MSE

is offering this reducing property and the concentration of this agent in the MSE.

(Authors’ Response) Thank you for reviewer comment. This is considered in revised version new section was inserted in introduction with some references explaining the potential reduction capability of molokhia extract and the compounds responsible for this action as listed.

Inserted Section

(Pages 2-3) Additionally, molokhia (Corchorus olitorius L.),  a well-known Egyptian vegetable also known as Egyptian spinach, is also grown in large quantities every year. Unexpectedly, it was discovered that molokhia extract has a wealth of beneficial phenolic and antioxidant chemicals such as such as vitamin C, vitamin E, β-carotene, α-tocopherol, glutathione, and phenols  [16-18] that have the potential to function as potential reducing agents to metal ions [19]. This is in addition of exitance of terpenoids which serve as capping for prepared metal nanoparticles [ 20-21].

 

 

 

Inserted references

[18] Azuma, K.; Nakayama, M.; Koshioka, M.; Ippoushi, K.; Yamaguchi, Y.; Kohata, K.; Yamauchi, Y.; Ito, H.; Higashio, H. Phenolic Antioxidants from the Leaves of Corchorus olitorius L. J. Agric. Food Chem. 1999, 47, 3963-3966.

[19] Ismail, E. H.; Saqer, A. M. A.; Assirey, E.; Arshi Naqvi, A.; Okasha, R. M. Successful green synthesis of gold nanoparticles using a corchorus olitorius extract and their antiproliferative effect in cancer cells. Int. J. Mol. Sci. 2018, 19, 2612.

[20] Haque, M. J.; Bellah, M. M.; Hassan, M. R.; Rahman, S. Synthesis of ZnO nanoparticles by two different methods comparison of their structural, antibacterial, photocatalytic and optical properties. Nano Express 2020, 1, 010007.

[21] Nath Roy, D. Terpenoids Against Human Diseases. CRC Press, Boca Raton, 2019.

 

 

2. More detailed synthetical mechanism of the ZnO NP should be provided, including the role of

elevating pH value, why use zinc acetate as the precursor for the sol-gel process, and the role

of oxygen in the ZnO formation process.

(Authors’ Response) Thank you for reviewer comment. This is considered in revised version and highlighted and new section was inserted with some references. Also, zinc acetate was used as precursor because it was the available Zinc salt available in Laboratory.

Inserted Section

(Page 5) Actually, once disperse MSE to zinc acetate solution the rich phenolic and antioxidant compounds [17-21]  exist the solution afford electron transfer to Zn ions and reduce Zn ions to ZnONPs which associated with change in color once reduction take place as represented in Fig. 1. Also, increase in pH value is critical to accomplish ZnONPs formation as it was fund that the existence of rich hydroxide ions is necessary for reactants to form nanoparticles [24-26].

Inserted References  

[24] Amin, G.; Asif, M. H.; Zainelabdin, A.; Zaman, S.; Nur, O.; M. Willander, M.

Influence of pH, precursor concentration, growth time, and temperature on the morphology of ZnO nanostructures grown by the hydrothermal method. J. Nanomaterial 2011,2011, 269692.

[25] Yang, L. L.; Zhao, Q. X.; M. Willander, M. Size-controlled growth of well-aligned ZnO nanorod arrays with two-step chemical bath deposition method

629. Alloys Compd. 2009, 469, 623-629.

[26] Alver, U.;  Kudret, A.; S. Kerli, S. Influence of pH on structural, optical and morphological properties of ZnO rod arrays fabricated by hydrothermal method

Opt. Adv. Mat. -Ra. Com., 2012, 6, 107-109.

 

3. How does starch help the ZnO NP to deposit onto hand embroidery thread? More explanation on the depositing process should be provided. Also, the MSE-ZnONP-ST is supposed to have a “core-shell” structure, but no such feature can be observed in Figure 2. The authors are encouraged to provide better TEM images and measure the shell size of the starch coating layer.

 

(Authors’ Response) Thank you for reviewer comment. This is considered in revised version and highlighted and new section was inserted with some references. As, the role starch for fixing the ZnONPs on the surface of cotton hand embroidery threads was clearly noticed on the formation of supramolecular interaction (hydrogen bonding) between hydroxyl group of starch and hydroxyl groups of cotton threads decorating the ZnONPs on the surface of cotton threads rather than incorporating inside the amorphous region and this was corroborated in positive tensile strength behavior. Actually, the starch layer wrapped the prepared ZnONPs can’t be visible seen as regular shell in TEM image as it is polymer in nature. However, we tried several times to take the image but it doesn’t work. Thus, the following section was inserted in revised version

 

 

Inserted Section

(Pages 5-6) It is noteworthy to note that, the coating layer composed from MSE-ZnONP-ST was interacted to  the cotton hand embroidery threads surfaces via supramolecular interaction (H-Boding). Thus, the rich hydroxyl groups exist on the structure of MSE and ST capped and wrapped the ZnONPs form dense hydrogen bonding with hydroxy groups of cotton hand embroidery threads [27-28]. Therefore, these strengthen the interaction of the coating layer based on ZnONPs with cotton threads. 

Inserted references  

[27] Attia, N. F.; Moussa, M.; Sheta, A. M. F.; Taha, R.; Gamal, H.  Effect of different nanoparticles based coating on the performance of textile properties. Prog. Org. Coat. 2017, 104, 72-80.

[28] Poon, C. K.;  Kan, C. K.  Effects of TiO2 and curing temperatures on flame retardant finishing of cotton. Carbohyd. Polym. 2017, 121, 457-467.

 

4. For Figure 4 SEM-EDS mapping images, it seemed like the elements were just randomly scattered over the observatory field. The authors may consider to overlay the mapping images over

the original SEM secondary electron image to better assign each element spot to an exact

structure of your specimen.

 (Authors’ Response) Thank you for reviewer comment. This is considered in revised version and highlighted and Figure 4 was modified as listed.

1. In Tensile test section, the authors summarized the tensile strength in a unit of N, since all the hand embroidery threads have different width, we may consider calculating the tensile strength in a unit of kPa for a better presentation and comparison of the results.

(Authors’ Response) Thank you for reviewer comment. Actually, the tensile strength was displayed in the unit of N as it is the maximum force at break and this was conducted based the standard test method implemented in this kind of thread measurement (Standard test method BS 1932: Part 2 Knot Strength of Yarn and Thread). Also, all hand embroidery threads have similar widths and length used.

2. For antibacterial test, the authors should also test the performance on Gram-negative bacteria

like E. coli, only one type of bacteria test does not formulate a compelling result.

Also, in Figure 5, there were too much variance in the size of the threads loaded for

the inhibitory zone test. The authors should use the same weight of thread for each sample and fold them into the same size then load onto culture plate.

 

(Authors’ Response) Thank you for reviewer comment. Actually, the samples of hand embroidery threads used for antibacterial tested were evaluated based on similar mass and length and then fold. Therefore, the clear inhibition zone attained for each sample was next of three-time culture. Also, we tried to order the E. coli as an example of gram-negative bacteria to test our developed coated threads, however, it will take long time longer than the review time.

 

3. Section 2.3 should be titled as “Preparation of coated hand embroidery threads” instead of

“Synthesis of hand embroidery threads coatings”.

 

(Authors’ Response) Thank you for reviewer comment. This was considered in revised version and

Synthesis of hand embroidery threads coatings was modified to Preparation of hand embroidery threads coatings highlighted.

8. There are two “and” neighboring to each other in Page 2 line 87, please delete one of them.

 

(Authors’ Response) Thank you for reviewer comment. This was considered in revised version.

 

 

 

Author Response File: Author Response.doc

Round 2

Reviewer 3 Report

The problem in previous version of the manuscript was well-addressed. I recommend accepting this manuscript in its present form.