Abstract

Purpose - This paper aims to study the thermal oxidation performance of antioxidant additives in ester base oils deeply.Design/methodology/approach - ReaxFF molecular dynamics was used to simulate the thermal oxidation process of butyl octyl diphenylamine and octadecyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl) propanoate as two antioxidant additives act on the Trimethylolpropane trioleate (TMPTO) base oil. Meanwhile, combining with the infrared spectroscopy characterization results of the thermal oxidation test, this paper provides theoretical support for the development of high-performance synthetic lubricants and their antioxidant additives.Findings - The results show that butyl octyldiphenylamine easily removes the hydrogen atom on the secondary amine, which promotes the formation of more long carbon chain diene radicals or polyene hydroperoxides from TMPTO. Octadecyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl) propanoate could easily decompose into octadecyl hydroperoxide and 2,6-di-tert-butyl 4-propionylphenol, which could convert into 2-tert-butyl-4-peroxyethyl-6-hydroperoxy-tert-butylphenol in the middle of the thermal oxidation reaction, prompting TMPTO to form more short-chain alkenyl and olefin hydroperoxide or other oxide.Originality/value - The main change characteristics of base oil molecules are the first thermal decomposition to form oleic acid groups and ethane cyclopropane methyl oleate. Under the action of butyl octyldiphenylamine and octadecyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl) propanoate, the deep oxidation and decomposition reaction are slowed down.Peer review The peer review history for this article is available at: https://publons.com/publon/10.1108/ILT-01-2020-0037/


Authors

Zhan, Wen;  Zhan, Shengpeng;  Duan, HaiTao;  Li, Xinxiang;  Li, Jian;  Cheng, Bingxue;  Yuan, Chengqing

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  • pre-publication peer review (FINAL ROUND)
    Decision Letter
    2020/03/17

    17-Mar-2020


    Dear Zhan, Wen; Zhan, Shengpeng; Duan, HaiTao ; Li, Xinxiang ; Li, Jian ; Cheng, Bingxue


    It is a pleasure to accept your manuscript ilt-01-2020-0037.R1, entitled "The thermal oxidation mechanism of TMPTO with antioxidants investigated by ReaxFF MD" in its current form for publication in Industrial Lubrication and Tribology. Please note, no further changes can be made to your manuscript.


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    Thank you for your contribution. On behalf of the Editors of Industrial Lubrication and Tribology, we look forward to your continued contributions to the Journal.


    Sincerely,
    Prof. Carsten Gachot
    Editor, Industrial Lubrication and Tribology
    carsten.gachot@tuwien.ac.at

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    Author Response
    2020/03/11

    Dear editer and reviewer :
    Its pleasure to hear about the recommend of my manuscript.Occording to reviewer comments. I have corrected manuscript. The details answers like thus.



    1. In the process of molecular dynamics simulation with ReaxFF force field, the author need to give the information including the size of the simulated model and some relevant references about potential parameters of ReaxFF force field.


    Answer: I would like to modify the last sentence of section 2.2, adding lattice parameter.also,other potential parameters save at section 2.1 ,like: The temperature cycle range, cycles optimization, The constant temperature, the integration step...


    As shown in Figure 2 and Figure 3 are respectively simulation results of lubricants B (lattice parameter 22.676 Å×22.676 Å×22.676 Å), lubricants C (lattice parameter 22.905 Å×22.905 Å×22.905 Å)




    1. In section 2.2, what is the meaning of “molecular crystalline state”? Generally, the lubricating oil is in amorphous state.
      Answer: “molecular crystalline” interpretate lattice. I would like to modiy in manuscript mark red.




    2. In the experimental section (section 2.3), the details of oxidation methods of lubricating oils need to be added.
      Answer: I would like to add that method at the first sentence of section 2.3 .
      Taking glass beaker filled with lubricants B/C in an oven to carry out accelerated thermal oxidation test, set the thermal oxidation cycle at 135°C for 15days, and regularly collect thermal lubricant samples




    3. In the analysis of infrared spectra, did the expressions of 3008 cm-1 and 3011 cm-1 express a same peak? If yes, you’d better to use one wavenumber. Besides, the author shows that the peak at 1660 did not change significantly and C=C bond was stable. Maybe it was because the infrared spectroscopy is not sensitive for the detection of C=C bond.
      Answer: The manuscript point out the local infrared spectra near 3008 cm-1 and 1660 cm-1-1527 cm-1 were taken weekly in lubricants B. but ,the phenomenon of lubricants C were changed significantly. We thought that it is not sensitive of IR. Please save our original opinion.




    4. In section 3.1, the author shows that the thermal oxidation reaction of the system is slow under the action of the antioxidant. What is your reference or standard for comparison? Have you done the simulation of TMPTO without the antioxidant?
      Answer: We also simulated reaction process of lubricating oil A for comparative results of number and type of molecules,and set up Thermal oxidation process o TMPTO in Fig 8. So that we could discusse the thermal oxidation mechanism of TMPTO with two antioxidants respectively.




    5. In section 3.2, the author used the expression of “compared with the change of lubricating oil A”. What is the meaning of “lubricating oil A”?
      Answer: A represents a sample of TMPTO. I would like to modify the sentence of section 2.2 mark red.




    6. In the section 3.4, the anti-oxidtive function of phenolic hydroxy of phenol antioxidant was seemingly not obtained in your simulation of lubricating oil C. As a radical scavenger, the phenolic hyroxy generally detaches its active hydrogen atom. It needs to be explained.
      Answer: Certainly, some relative phenol antioxidant was reported that radical scavenger could be detached its active hydrogen atom. But also ,there are out of evidence. In my research ,we get the reaction process of phenol antioxidant Octadecyl 3-(3,5-di-tert-butyl-4-hydroxyphenyl)propanoate with base oil TMPTO in FIG 9. It is show the main mechanism of action of antioxidants.①The antioxidant is firstly decomposed into octadecyl hydroperoxide and 2,6-di-tert-butyl-4-propionic phenol group,which also detached its active hydrogen atom. What`more, ②The 2,6-di-tert-butyl-4-ethyl-phenol radical transition state immediately formed is beneficial to the lubricating oil to maintain its oxidation resistance under low temperature conditions.




    Best regards to you!
    Wen Zhan



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  • pre-publication peer review (ROUND 1)
    Decision Letter
    2020/03/08

    08-Mar-2020


    Dear Dr. Zhan:


    Manuscript ID ilt-01-2020-0037 entitled "The thermal oxidation mechanism of TMPTO with antioxidants investigated by ReaxFF MD" which you submitted to the Industrial Lubrication and Tribology, has been reviewed. The comments of the reviewer(s) are included at the bottom of this letter.


    The reviewer(s) have recommended revisions to the submitted manuscript, before it can be considered for publication. Therefore, I invite you to respond to the reviewer(s)' comments and revise your manuscript.


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    Once again, thank you for submitting your manuscript to the Industrial Lubrication and Tribology and I look forward to receiving your revision.


    Sincerely,
    Prof. Carsten Gachot
    Editor, Industrial Lubrication and Tribology
    carsten.gachot@tuwien.ac.at


    Reviewer(s)' Comments to Author:
    Reviewer: 1


    Comments to the Author
    This paper investigated the oxidation behavior of TMPTO oil involving the amine or phenol antioxidant using the experimental analysis and molecular dynamics simulation. The complicated oxidation process of TMPTO and the function of antioxidatnts were obtained. Before formal acceptance, some questions need to be improved for clarity.




    1. In the process of molecular dynamics simulation with ReaxFF force field, the author need to give the information including the size of the simulated model and some relevant references about potential parameters of ReaxFF force field.




    2. In section 2.2, what is the meaning of “molecular crystalline state”? Generally, the lubricating oil is in amorphous state.




    3. In the experimental section (section 2.3), the details of oxidation methods of lubricating oils need to be added.




    4. In the analysis of infrared spectra, did the expressions of 3008 cm-1 and 3011 cm-1 express a same peak? If yes, you’d better to use one wavenumber. Besides, the author shows that the peak at 1660 did not change significantly and C=C bond was stable. Maybe it was because the infrared spectroscopy is not sensitive for the detection of C=C bond.




    5. In section 3.1, the author shows that the thermal oxidation reaction of the system is slow under the action of the antioxidant. What is your reference or standard for comparison? Have you done the simulation of TMPTO without the antioxidant?




    6. In section 3.2, the author used the expression of “compared with the change of lubricating oil A”. What is the meaning of “lubricating oil A”?




    7. In the section 3.4, the anti-oxidtive function of phenolic hydroxy of phenol antioxidant was seemingly not obtained in your simulation of lubricating oil C. As a radical scavenger, the phenolic hyroxy generally detaches its active hydrogen atom. It needs to be explained.




    Reviewer: 2


    Comments to the Author
    (There are no comments.)
    Reviewer: 1


    Comments:
    This paper investigated the oxidation behavior of TMPTO oil involving the amine or phenol antioxidant using the experimental analysis and molecular dynamics simulation. The complicated oxidation process of TMPTO and the function of antioxidatnts were obtained. Before formal acceptance, some questions need to be improved for clarity.




    1. In the process of molecular dynamics simulation with ReaxFF force field, the author need to give the information including the size of the simulated model and some relevant references about potential parameters of ReaxFF force field.




    2. In section 2.2, what is the meaning of “molecular crystalline state”? Generally, the lubricating oil is in amorphous state.




    3. In the experimental section (section 2.3), the details of oxidation methods of lubricating oils need to be added.




    4. In the analysis of infrared spectra, did the expressions of 3008 cm-1 and 3011 cm-1 express a same peak? If yes, you’d better to use one wavenumber. Besides, the author shows that the peak at 1660 did not change significantly and C=C bond was stable. Maybe it was because the infrared spectroscopy is not sensitive for the detection of C=C bond.




    5. In section 3.1, the author shows that the thermal oxidation reaction of the system is slow under the action of the antioxidant. What is your reference or standard for comparison? Have you done the simulation of TMPTO without the antioxidant?




    6. In section 3.2, the author used the expression of “compared with the change of lubricating oil A”. What is the meaning of “lubricating oil A”?




    7. In the section 3.4, the anti-oxidtive function of phenolic hydroxy of phenol antioxidant was seemingly not obtained in your simulation of lubricating oil C. As a radical scavenger, the phenolic hyroxy generally detaches its active hydrogen atom. It needs to be explained.




    Additional Questions:
    Originality: Does the paper contain new and significant information adequate to justify publication?: yes, but before formal acceptance, some questions need to be improved for clarity


    Relationship to Literature: Does the paper demonstrate an adequate understanding of the relevant literature in the field and cite an appropriate range of literature sources? Is any signficant work ignored?: yes


    Methodology: Is the paper's argument built on an appropriate base of theory, concepts, or other ideas? Has the research or equivalent intellectual work on which the paper is based been well designed? Are the methods employed appropriate?: yes, but some questions need to answer.


    Results: Are results presented clearly and analysed appropriately? Do the conclusions adequately tie together the other elements of the paper?: yes


    Practicality and/or Research implications: Does the paper identify clearly any implications for practice and/or further research? Are these implications consistent withthe findings and conclusions of the paper?: yes


    Quality of Communication: Does the paper clearly express its case, measured against the technical language of the field and the expected knowledge of the journal's readership? Has attention been paid to the clarity of expression and readability, such as sentence structure, jargon use, acronyms, etc.: yes


    Reproducible Research: If appropriate, is sufficient information, potentially including data and software, provided to reproduce the results and are the corresponding datasets formally cited?: yes, but some areas need minor repairs


    This journal is participating in Publons Transparent Peer Review. By reviewing for this journal, you agree that your finished report, along with the author’s responses and the Editor’s decision letter, will be linked to from the published article to where they appear on Publons, if the paper is accepted. If you have any concerns about participating in the Transparent Peer Review pilot, please reach out to the journal’s Editorial office. Please indicate below, whether you would like your name to appear with your report on Publons by indicating yes or no: Yes, I would like my name to appear with my report on Publons


    Reviewer: 2


    Comments:
    (There are no comments.)


    Additional Questions:
    Originality: Does the paper contain new and significant information adequate to justify publication?: Yes, it is.


    Relationship to Literature: Does the paper demonstrate an adequate understanding of the relevant literature in the field and cite an appropriate range of literature sources? Is any signficant work ignored?: The paper demonstrate an adequate experiment such as the ReaxFF moculular dynamics to stimulate thermal oxidation process of Butyl Octyl Diphenylamine and octadecyl3- etc.
    There is no significant work to be ignored.


    Methodology: Is the paper's argument built on an appropriate base of theory, concepts, or other ideas? Has the research or equivalent intellectual work on which the paper is based been well designed? Are the methods employed appropriate?: The paper has been built up their own idea to demonstrate the effect of two antioxidant addivies on the TMPTO base oil. It was employed appropriate.


    Results: Are results presented clearly and analysed appropriately? Do the conclusions adequately tie together the other elements of the paper?: Yes, the results presented clearly.


    Practicality and/or Research implications: Does the paper identify clearly any implications for practice and/or further research? Are these implications consistent withthe findings and conclusions of the paper?: Yes, the implications consitstent with the findings and conclusions.


    Quality of Communication: Does the paper clearly express its case, measured against the technical language of the field and the expected knowledge of the journal's readership? Has attention been paid to the clarity of expression and readability, such as sentence structure, jargon use, acronyms, etc.: Yes, the quality of communication is good for the paper.


    Reproducible Research: If appropriate, is sufficient information, potentially including data and software, provided to reproduce the results and are the corresponding datasets formally cited?: Yes, they showed proper datasets with the citation.


    This journal is participating in Publons Transparent Peer Review. By reviewing for this journal, you agree that your finished report, along with the author’s responses and the Editor’s decision letter, will be linked to from the published article to where they appear on Publons, if the paper is accepted. If you have any concerns about participating in the Transparent Peer Review pilot, please reach out to the journal’s Editorial office. Please indicate below, whether you would like your name to appear with your report on Publons by indicating yes or no: No, I would not like my name to appear with my report on Publons

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    Reviewer report
    2020/03/01

    This paper investigated the oxidation behavior of TMPTO oil involving the amine or phenol antioxidant using the experimental analysis and molecular dynamics simulation. The complicated oxidation process of TMPTO and the function of antioxidatnts were obtained. Before formal acceptance, some questions need to be improved for clarity.

    1. In the process of molecular dynamics simulation with ReaxFF force field, the author need to give the information including the size of the simulated model and some relevant references about potential parameters of ReaxFF force field.

    2. In section 2.2, what is the meaning of “molecular crystalline state”? Generally, the lubricating oil is in amorphous state.

    3. In the experimental section (section 2.3), the details of oxidation methods of lubricating oils need to be added.

    4. In the analysis of infrared spectra, did the expressions of 3008 cm-1 and 3011 cm-1 express a same peak? If yes, you’d better to use one wavenumber. Besides, the author shows that the peak at 1660 did not change significantly and C=C bond was stable. Maybe it was because the infrared spectroscopy is not sensitive for the detection of C=C bond.

    5. In section 3.1, the author shows that the thermal oxidation reaction of the system is slow under the action of the antioxidant. What is your reference or standard for comparison? Have you done the simulation of TMPTO without the antioxidant?

    6. In section 3.2, the author used the expression of “compared with the change of lubricating oil A”. What is the meaning of “lubricating oil A”?

    7. In the section 3.4, the anti-oxidtive function of phenolic hydroxy of phenol antioxidant was seemingly not obtained in your simulation of lubricating oil C. As a radical scavenger, the phenolic hyroxy generally detaches its active hydrogen atom. It needs to be explained.

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