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Title: The Role of Transition Metals on Chemo-Mechanical Instabilities in Prussian Blue Analogues For K-Ion Batteries: The Case Study on KNHCF Versus KMHCF

Abstract

Prussian blue analogues (PBAs) cathodes can host diverse monovalent and multivalent metal ions due to their tunable structure. However, their electrochemical performance suffers from poor cycle life associated with chemo-mechanical instabilities. This study investigates the driving forces behind chemo-mechanical instabilities in Ni- and Mn-based PBAs cathodes for K-ion batteries by combining electrochemical analysis, digital image correlation, and spectroscopy techniques. Capacity retention in Ni-based PBA is 96% whereas it is 91.5% for Mn-based PBA after 100 cycles at C/5 rate. During charge, the potassium nickel hexacyanoferrate (KNHCF) electrode experiences a positive strain generation whereas the potassium manganese hexacyanoferrate (KMHCF) electrode undergoes initially positive strain generation followed by a reduction in strains at a higher state of charge. Overall, both cathodes undergo similar reversible electrochemical strains in each charge–discharge cycle. There is ~0.80% irreversible strain generation in both cathodes after 5 cycles. XPS studies indicated richer organic layer compounds in the cathode-electrolyte interface (CEI) layer formed on KMHCF cathodes compared to the KNHCF ones. Faster capacity fades in Mn-based PBA, compared to Ni-based ones, is attributed to the formation of richer organic compounds in CEI layers, rather than mechanical deformations. In conclusion, understanding the driving forces behind instabilities provides a guideline tomore » develop material-based strategies for better electrochemical performance.« less

Authors:
 [1];  [2];  [2];  [3];  [4];  [4];  [4]; ORCiD logo [3];  [4]; ORCiD logo [2]
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  1. Purdue Univ., West Lafayette, IN (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  2. Oklahoma State Univ., Stillwater, OK (United States)
  3. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  4. Purdue Univ., West Lafayette, IN (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of Maryland Baltimore County (UMBC), Baltimore, MD (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
2202417
Alternate Identifier(s):
OSTI ID: 1995882; OSTI ID: 2281649
Report Number(s):
PNNL-SA-179465
Journal ID: ISSN 1614-6832
Grant/Contract Number:  
AC05-76RL01830; SC0021251; CBET-1804300; DMR-2016453
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 13; Journal Issue: 32; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Prussian blue analogues; XPS; cathode-electrolyte interface; strain; mechanical deformation

Citation Formats

Li, Zheng, Ozdogru, Bertan, Bal, Batuhan, Bowden, Mark, Choi, Austin, Zhang, Yizhi, Wang, Haiyan, Murugesan, Vijayakumar, Pol, Vilas G., and Çapraz, Ömer Özgür. The Role of Transition Metals on Chemo-Mechanical Instabilities in Prussian Blue Analogues For K-Ion Batteries: The Case Study on KNHCF Versus KMHCF. United States: N. p., 2023. Web. doi:10.1002/aenm.202301329.
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Li, Zheng, Ozdogru, Bertan, Bal, Batuhan, Bowden, Mark, Choi, Austin, Zhang, Yizhi, Wang, Haiyan, Murugesan, Vijayakumar, Pol, Vilas G., & Çapraz, Ömer Özgür. The Role of Transition Metals on Chemo-Mechanical Instabilities in Prussian Blue Analogues For K-Ion Batteries: The Case Study on KNHCF Versus KMHCF. United States. https://doi.org/10.1002/aenm.202301329
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Li, Zheng, Ozdogru, Bertan, Bal, Batuhan, Bowden, Mark, Choi, Austin, Zhang, Yizhi, Wang, Haiyan, Murugesan, Vijayakumar, Pol, Vilas G., and Çapraz, Ömer Özgür. Mon . "The Role of Transition Metals on Chemo-Mechanical Instabilities in Prussian Blue Analogues For K-Ion Batteries: The Case Study on KNHCF Versus KMHCF". United States. https://doi.org/10.1002/aenm.202301329.
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@article{osti_2202417,
title = {The Role of Transition Metals on Chemo-Mechanical Instabilities in Prussian Blue Analogues For K-Ion Batteries: The Case Study on KNHCF Versus KMHCF},
author = {Li, Zheng and Ozdogru, Bertan and Bal, Batuhan and Bowden, Mark and Choi, Austin and Zhang, Yizhi and Wang, Haiyan and Murugesan, Vijayakumar and Pol, Vilas G. and Çapraz, Ömer Özgür},
abstractNote = {Prussian blue analogues (PBAs) cathodes can host diverse monovalent and multivalent metal ions due to their tunable structure. However, their electrochemical performance suffers from poor cycle life associated with chemo-mechanical instabilities. This study investigates the driving forces behind chemo-mechanical instabilities in Ni- and Mn-based PBAs cathodes for K-ion batteries by combining electrochemical analysis, digital image correlation, and spectroscopy techniques. Capacity retention in Ni-based PBA is 96% whereas it is 91.5% for Mn-based PBA after 100 cycles at C/5 rate. During charge, the potassium nickel hexacyanoferrate (KNHCF) electrode experiences a positive strain generation whereas the potassium manganese hexacyanoferrate (KMHCF) electrode undergoes initially positive strain generation followed by a reduction in strains at a higher state of charge. Overall, both cathodes undergo similar reversible electrochemical strains in each charge–discharge cycle. There is ~0.80% irreversible strain generation in both cathodes after 5 cycles. XPS studies indicated richer organic layer compounds in the cathode-electrolyte interface (CEI) layer formed on KMHCF cathodes compared to the KNHCF ones. Faster capacity fades in Mn-based PBA, compared to Ni-based ones, is attributed to the formation of richer organic compounds in CEI layers, rather than mechanical deformations. In conclusion, understanding the driving forces behind instabilities provides a guideline to develop material-based strategies for better electrochemical performance.},
doi = {10.1002/aenm.202301329},
journal = {Advanced Energy Materials},
number = 32,
volume = 13,
place = {United States},
year = {Mon Jul 24 00:00:00 EDT 2023},
month = {Mon Jul 24 00:00:00 EDT 2023}
}
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https://doi.org/10.1002/aenm.202301329
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