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

Li, Zheng; Ozdogru, Bertan; Bal, Batuhan; Bowden, Mark; Choi, Austin; Zhang, Yizhi; Wang, Haiyan; Murugesan, Vijayakumar; Pol, Vilas G.; Çapraz, Ömer Özgür

doi:10.1002/aenm.202301329

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

Journal Article · Mon Jul 24 00:00:00 EDT 2023 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202301329· OSTI ID:2202417

Li, Zheng ^[1]; Ozdogru, Bertan ^[2]; Bal, Batuhan ^[2]; Bowden, Mark ^[3]; Choi, Austin ^[4]; Zhang, Yizhi ^[4]; Wang, Haiyan ^[4];

^[3]; Pol, Vilas G. ^[4];

^[2]

Purdue Univ., West Lafayette, IN (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Oklahoma State Univ., Stillwater, OK (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Purdue Univ., West Lafayette, IN (United States)

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.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of Maryland Baltimore County (UMBC), Baltimore, MD (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC05-76RL01830; SC0021251; CBET-1804300; DMR-2016453

OSTI ID:: 2202417

Alternate ID(s):: OSTI ID: 1995882; OSTI ID: 2281649

Report Number(s):: PNNL-SA-179465

Journal Information:: Advanced Energy Materials, Vol. 13, Issue 32; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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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

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