Review of Aging Mechanism and Diagnostic Methods for Lithium-Ion Batteries

Round 1

Reviewer 1 Report

Comments and Suggestions for Authors

The manuscript contains a broad collection of works related to the mechanisms of aging diagnosis in lithium-ion batteries; however, some points should be considered.

1. I think it is appropriate to include the specific capacities of these batteries as an introduction, at least those listed as examples.
2. Although it describes some structural and morphological characterization techniques, etc., and mentions some articles as examples, there is no discussion or connection with a tangible electrochemical result. For example, how phase change affects battery performance in the material indicated in the text. Each of the examples provided should be supported by the electrochemical section to see how this aspect affects.
3. There are many errors in the subscripts of the chemical compounds.
4. Most of the images are very small, and it is not possible to appreciate what they highlight in the manuscript.
5. Too much typo error.

Author Response

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Reviewer 2 Report

Comments and Suggestions for Authors

This manuscript provides a general review of the aging mechanisms and diagnostic methods for lithium-ion batteries. While it offers a brief overview of various analytical techniques and presents several representative aging mechanisms along with diagnostic processes, the discussion of these techniques remains largely descriptive rather than being organically integrated from a diagnostic perspective. Moreover, the logical flow and structural consistency of the manuscript are insufficient. The authors’ intention to incorporate diagnostic approaches from other research domains is meaningful; however, the manuscript does not convincingly demonstrate the effectiveness or applicability of such methods in the context of lithium-ion battery diagnostics. In addition, numerous typographical and formatting issues, such as subscript errors, incorrect capitalization, inappropriate hyphenation, and the frequent use of unexplained abbreviations without first presenting their full terms, significantly impair the readability of the text. The categorization of anode LAM and cathode LAM is presented in an almost identical manner, offering little insight into the differences in aging mechanisms. As a result, the classification system does not effectively offer readers deeper insights or practical implications. Given these limitations, the manuscript is unlikely to appeal to a broader readership and, regrettably, does not meet the standards expected for publication in this journal, particularly in light of efforts to enhance its academic prestige.

The authors' intention to integrate diagnostic approaches from other research areas is meaningful. However, the manuscript does not convincingly demonstrate the effectiveness or applicability of such methods in the context of lithium-ion battery diagnostics.

Author Response

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Reviewer 3 Report

Comments and Suggestions for Authors

energies-3691215; review report

 

Paper Title: Review of Aging Mechanism and Diagnostic Methods for Lithium-ion Batteries

Authors presented a review of aging mechanism of lithium-ion batteries and diagnostic methods for lithium-ion battery aging. Authors reviewed li-ion battery aging mechanisms, macroscopic and microscopic methods of battery aging analysis, and specific diagnostic protocols for each aging mechanism, and diagnostic process and development trend. My comments are as follows.

 

1. The strong point of the manuscript is its comprehensiveness. The manuscript, however, has some weak points.

1) Microscopic methods may be better categorized as methods of battery aging research than as diagnostic methods. They are laboratory-based methods that is difficult to be implemented as a part of implementable battery-aging diagnostic methods. In Abstract, authors stated "Finally, combined with macroscopic and microscopic diagnosis methods, it systematically summarizes a highly universal standardized routine diagnosis process for battery aging."

Please consider restructuring the paper differentiating between implementable methods and laboratory techniques. Please also consider revising the paper title accordingly.

2) Authors cited many research works without analyzing their effectiveness or merits.

Borrowing from food technologies seems to be too vague and not to the point. For example, in Lines 69-73, authors wrote "Temperature control and environmental monitoring are also important to maintain food freshness, which is similar to the temperature management of lithium-ion batteries during operation. By drawing on the monitoring technology of cold chain logistics, a new perspective can be provided for the aging diagnosis of lithium-ion batteries [7]." In the same line, '5.2.3 Learn from multiple fields' should be a laboratory research method for understanding battery aging mechanism rather than an approach for diagnosis.

3) '5.2.4 Vehicle-cloud data fusion'

 Is it really necessary to employ the cloud computer for battery aging diagnosis? The prediction of battery aging (for example in electric vehicles) needs not to be highly accurate. In many cases, a simple embedded algorithm should be enough. The use of the cloud computing would be better suited for research and in  algorithm development stages.

3. '6 Summing-up' needs to be expanded judging from the extensive scope of the paper.
4. In Lines 1022-1026, authors wrote "Additionally, based on Kennards-Stone (KS) and Soft Independent Modeling with Clustering (SIMCA), the prediction accuracy is perfect. Therefore, the GC-IMS system demonstrates to be an effective method for classifying edible plant oils, and similar methods can also be used to classify vehicles at the cloud platform level[140]."

Please check these statements, especially '...perfect.' and '...to classify vehicles...'.

Author Response

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Reviewer 4 Report

Comments and Suggestions for Authors

This review is valuable paper for publishing in this journal. However, there are a few issues, which is subjected to a minor revision.

1. What's the "dual carbon" policy? Explanation and citation should be included for readership.
2. Initial coulombic efficiency is an importan factor for aging and formation. Some discussion should be included.
3. XPS is also a useful method for aging and SEI and CEI study, which should be reviewed.
4. Aging and formation is an important operation for LIB manufacturing (Advanced electrode processing for lithium-ion battery manufacturing), especially at electrode level and cell level, and it is suggested to have some discussion based on aspect of LIB manufacturing. The authors should check and discuss the pioneering literature listed above. 
5. The English writing should be polished. 
6. What's the impact of aging on anode SEI and cathode CEI?

Author Response

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Reviewer 5 Report

Comments and Suggestions for Authors

This manuscript presents a review of mechanisms of lithium battery aging and the methods used for diagnosing aging. Nevertheless, there are some issues that need to be addressed. In particular, there are conceptual inaccuracies in the characterization sections. Moreover, the diagnostic techniques are not clearly linked to battery aging. Instead, they are introduced in a way that resembles a general overview, as one might find in the introduction of a PhD thesis, rather than being critically discussed in the context of the aging mechanism.

1. When the authors introduce the characterization methods, they do not effectively relate these techniques to their applications in battery studies. Instead, they provide some background information that is somewhat disconnected or even misleading. For instance, it should be mentioned that operando XRD can monitor real-time structural evolution during cycling, and ex situ XRD can reveal the crystalline structure of active materials after hundreds of cycles.

There are quite a few types and inconsistencies in the use of capital and lowcase letters that should be corrected. For instance, please change “x-ray diffraction” to X-ray diffraction, and “neutron diffraction” to “Neutron diffraction”.

2. From Lines 391 to 406, the authors appear to describe X-ray absorption spectroscopy (XAS), but they incorrectly refer to it as “expand the X-ray fine spectrum”. This terminology is misleading. It should be clearly stated that XAS includes two main regions: X-ray near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS). In fact, XANES provides information on the local electronic structure and oxidation states of the target element, whereas EXAFS provides insights into the local atomic coordination. The current description in the manuscript reflects some conceptual misunderstandings that should be corrected.
3. In the case of the neutron diffraction section, ND and XRD indeed are useful for probing the structure of materials. Nevertheless, in battery research, a key distinction is that neutron diffraction is particularly suitable for detecting light atoms such as H and Li, and can, in some cases, even quantify their content.
4. In Lines 427 and 460, the authors should correct the title to “Raman spectroscopy”.

 

Author Response

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Round 2

Reviewer 2 Report

Comments and Suggestions for Authors

The authors have addressed the reviewers’ comments by correcting the noted issues in expression and distinguishing between anode and cathode diagnostics in diagnostic mode. They also provide valuable guidelines for diagnostic methodologies. Therefore, this manuscript can be recommended for publication.

Author Response

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Reviewer 5 Report

Comments and Suggestions for Authors

This review provides an overview of the battery aging mechanism, along with relevant macroscopic and microscopic diagnostic methods. The authors have made substantial revisions to the manuscript. However, there are still some issues that need to be addressed.

1. Indeed, the OCV test is closely related to the battery’s state of charge. In fact, you can also compare OCV values measured at two different time points and use the following equation to calculate the K value, which can help evaluate battery fading or internal particle-related self-charge: K=(OCV2-OCV1)/(t2-t1).
2. In Figure 5, please indicate the specific literature sources you have cited. The descriptions provided are very unclear, especially for Figure 5A. Additionally, the font size within the figure is too tiny to read. Please kindly revise all unclear or poorly formatted figures to ensure they are presented clearly.
3. XANES cannot determine the elemental composition. You should probe one element by tuning to its absorption edge. In fact, it is an element-specific technique for investigating the local structure rather than morphology. Please integrate XANES and EXAFS into a single section titled 'X-ray Absorption Spectroscopy'.
4. The authors do not need to provide detailed introductions to these characterization techniques, as they are commonly used in a wide range of scientific research beyond battery aging studies. If you include them in the manuscript, please integrate the discussion directly with the relevance to battery aging diagnostics, rather than presenting them in a single but long section.
5. Please ensure proper use of capitalization as well as accurate formatting of superscripts and subscripts. If you choose to capitalize each word in headings, please maintain this style consistently across the entire document.

Furthermore, please carefully check the typographical and grammatical errors throughout the manuscript.

Author Response

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Round 3

Reviewer 5 Report

Comments and Suggestions for Authors

The authors have addressed most of my previous suggestions. Nonetheless, a few detailed issues still need to be corrected.

1. In Figure 6, it would be more accurate to change “changes in material crystal structure” to “changes in material structure”. Furthermore, you might consider adding “XAS” under the subtitle named “Elements and valence states”.
2. Since you used “Scanning Tunnelling Microscopy” as a section title, it would be more consistent to also use the full names of other techniques, such as “Atomic Force Microscopy”, “Scanning Electron Microscopy”, and “Transmission Electron Microscopy” as section titles as well. Please note that microscopy is a technique, while a microscope is a physical instrument.

Author Response

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