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Title: Composition Dependent Electrochemical Properties of Earth-Abundant Ternary Nitride Anodes

Journal Article · · APL Materials
DOI:https://doi.org/10.1063/5.0083998· OSTI ID:1866074

Growing energy storage demands on lithium-ion batteries necessitate exploration of new electrochemical materials as next-generation battery electrode materials. In this work, we investigate the previously unexplored electrochemical properties of earth-abundant and tunable Zn 1−x Sn 1+x N 2 (x = −0.4 to x = 0.4) thin films, which show high electrical conductivity and high gravimetric capacity for Li insertion. Enhanced cycling performance is achieved compared to previously published end-members Zn 3 N 2 and Sn 3 N 4 , showing decreased irreversible loss and increased total capacity and cycle stability. The average reversible capacity observed is >1050 mAh/g for all compositions and 1220 mAh/g for Zn-poor (x = 0.2) films. Extremely Zn-rich films (x = −0.4) show improved adhesion; however, Zn-rich films undergo a phase transformation on the first cycle. Zn-poor and stoichiometric films do not exhibit significant phase transformations which often plague nitride materials and show no required overpotential at the 0.5 V plateau. Cation composition x is explored as a mechanism for tuning relevant mechanical and electrochemical properties, such as capacity, overpotential, phase transformation, electrical conductivity, and adhesion. The lithiation/delithiation experiments confirm the reversible electrochemical reactions. Without any binding additives, the as-deposited electrodes delaminate resulting in fast capacity degradation. We demonstrate the mechanical nature of this degradation through decreased electrode thinning, resulting in cells with improved cycling stability due to increased mechanical stability. Combining composition and electrochemical analysis, this work demonstrates for the first time composition dependent electrochemical properties for the ternary Zn 1−x Sn 1+x N 2 and proposes earth-abundant ternary nitride anodes for increased reversible capacity and cycling stability.

Research Organization:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); University of Colorado
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
1866074
Alternate ID(s):
OSTI ID: 1863133
Report Number(s):
NREL/JA-5K00-81808; MainId:82581; UUID:dd5e8891-d039-4d25-b965-b1d386267eb7; MainAdminID:64114; TRN: US2306555
Journal Information:
APL Materials, Vol. 10, Issue 4; ISSN 2166-532X
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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