Thermodynamically Driven Synthetic Optimization for Cation-Disordered Rock Salt Cathodes
Abstract
Relating the synthesis conditions of materials to their functional performance has long been an experience-based trial-and-error process. However, this methodology is not always efficient in identifying an appropriate protocol and can lead to overlooked opportunities for the performance optimization of materials through simple modifications of the synthesis process. In this work, we systematically track the structural evolution in the synthesis of a representative disordered rocksalt (a promising next-generation Li-ion cathode material) at the scale of both the long-range crystal structure and the short-range atomic structure using various in situ and ex situ techniques, including transmission electron microscopy, X-ray diffraction, and pair distribution function analysis. Further, an optimization strategy is proposed for the synthesis protocol, leading to a remarkably enhanced capacity (specific energy) of 313 mAh g–1 (987 Wh kg–1) at a low rate (20 mA g–1), with a capacity of more than 140 mAh g–1 retained even at a very high cycling rate of 2,000 mA g–1. This strategy is further rationalized using ab initio calculations, and important opportunities for synthetic optimization demonstrated in this study are highlighted.
- Authors:
-
[1];
[3];
[1];
[4];
[1];
[1]
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); University of Chinese Academy of Sciences, Beijing (China)
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Publication Date:
- Research Org.:
- Stony Brook Univ., NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). The Molecular Foundry (TMF) and National Energy Research Scientific Computing Center (NERSC); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Energy Frontier Research Centers (EFRC) (United States). Next Generation Synthesis Center (GENESIS); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1865715
- Alternate Identifier(s):
- OSTI ID: 1863455; OSTI ID: 1909701; OSTI ID: 1963446
- Grant/Contract Number:
- SC0019212; AC02-05CH11231; AC02-06CH11357; ACI1053575; DE‐AC02‐05CH11231; DE‐AC02‐06CH11357; AC02-05-CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Energy Materials
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 21; Related Information: aenm202103923-sup-0001-SuppMat.pdf; Journal ID: ISSN 1614-6832
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; disordered rock salts; Li-ion batteries; short-range order; synthesis science
Citation Formats
Cai, Zijian, Zhang, Ya‐Qian, Lun, Zhengyan, Ouyang, Bin, Gallington, Leighanne C., Sun, Yingzhi, Hau, Han‐Ming, Chen, Yu, Scott, Mary C., and Ceder, Gerbrand. Thermodynamically Driven Synthetic Optimization for Cation-Disordered Rock Salt Cathodes. United States: N. p., 2022.
Web. doi:10.1002/aenm.202103923.
Cai, Zijian, Zhang, Ya‐Qian, Lun, Zhengyan, Ouyang, Bin, Gallington, Leighanne C., Sun, Yingzhi, Hau, Han‐Ming, Chen, Yu, Scott, Mary C., & Ceder, Gerbrand. Thermodynamically Driven Synthetic Optimization for Cation-Disordered Rock Salt Cathodes. United States. https://doi.org/10.1002/aenm.202103923
Cai, Zijian, Zhang, Ya‐Qian, Lun, Zhengyan, Ouyang, Bin, Gallington, Leighanne C., Sun, Yingzhi, Hau, Han‐Ming, Chen, Yu, Scott, Mary C., and Ceder, Gerbrand. Sun .
"Thermodynamically Driven Synthetic Optimization for Cation-Disordered Rock Salt Cathodes". United States. https://doi.org/10.1002/aenm.202103923. https://www.osti.gov/servlets/purl/1865715.
@article{osti_1865715,
title = {Thermodynamically Driven Synthetic Optimization for Cation-Disordered Rock Salt Cathodes},
author = {Cai, Zijian and Zhang, Ya‐Qian and Lun, Zhengyan and Ouyang, Bin and Gallington, Leighanne C. and Sun, Yingzhi and Hau, Han‐Ming and Chen, Yu and Scott, Mary C. and Ceder, Gerbrand},
abstractNote = {Relating the synthesis conditions of materials to their functional performance has long been an experience-based trial-and-error process. However, this methodology is not always efficient in identifying an appropriate protocol and can lead to overlooked opportunities for the performance optimization of materials through simple modifications of the synthesis process. In this work, we systematically track the structural evolution in the synthesis of a representative disordered rocksalt (a promising next-generation Li-ion cathode material) at the scale of both the long-range crystal structure and the short-range atomic structure using various in situ and ex situ techniques, including transmission electron microscopy, X-ray diffraction, and pair distribution function analysis. Further, an optimization strategy is proposed for the synthesis protocol, leading to a remarkably enhanced capacity (specific energy) of 313 mAh g–1 (987 Wh kg–1) at a low rate (20 mA g–1), with a capacity of more than 140 mAh g–1 retained even at a very high cycling rate of 2,000 mA g–1. This strategy is further rationalized using ab initio calculations, and important opportunities for synthetic optimization demonstrated in this study are highlighted.},
doi = {10.1002/aenm.202103923},
journal = {Advanced Energy Materials},
number = 21,
volume = 12,
place = {United States},
year = {Sun Apr 17 00:00:00 EDT 2022},
month = {Sun Apr 17 00:00:00 EDT 2022}
}
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