Design principles for NASICON super-ionic conductors

Wang, Jingyang; He, Tanjin; Yang, Xiaochen; Cai, Zijian; Wang, Yan; Lacivita, Valentina; Kim, Haegyeom; Ouyang, Bin; Ceder, Gerbrand

doi:10.1038/s41467-023-40669-0

Design principles for NASICON super-ionic conductors

Journal Article · Fri Aug 25 00:00:00 EDT 2023 · Nature Communications

DOI:https://doi.org/10.1038/s41467-023-40669-0· OSTI ID:2281681

Wang, Jingyang ^[1]; ^[2]; Yang, Xiaochen ^[2]; ^[2]; ^[3]; Lacivita, Valentina ^[3]; Kim, Haegyeom ^[4]; Ouyang, Bin ^[5]; ^[2]

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States); Nanjing Univ., Suzhou (China)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Samsung Advanced Institute of Technology and Samsung Semiconductor, Inc, Cambridge, MA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Florida State Univ., Tallahassee, FL (United States)

Na Super Ionic Conductor (NASICON) materials are an important class of solid-state electrolytes owing to their high ionic conductivity and superior chemical and electrochemical stability. In this paper, we combine first-principles calculations, experimental synthesis and testing, and natural language-driven text-mined historical data on NASICON ionic conductivity to achieve clear insights into how chemical composition influences the Na-ion conductivity. These insights, together with a high-throughput first-principles analysis of the compositional space over which NASICONs are expected to be stable, lead to the successful synthesis and electrochemical investigation of several new NASICONs solid-state conductors. Among these, a high ionic conductivity of 1.2 mS cm^₋1 could be achieved at 25 °C. We find that the ionic conductivity increases with average metal size up to a certain value and that the substitution of PO₄ polyanions by SiO₄ also enhances the ionic conductivity. While optimal ionic conductivity is found near a Na content of 3 per formula unit, the exact optimum depends on other compositional variables. Surprisingly, the Na content enhances the ionic conductivity mostly through its effect on the activation barrier, rather than through the carrier concentration. These deconvoluted design criteria may provide guidelines for the design of optimized NASICON conductors.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); National Renewable Energy Laboratory (NREL), Golden, CO (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)

Grant/Contract Number:: AC02-05CH11231; SC0012704

OSTI ID:: 2281681

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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