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Title: Origin of anomalous high-rate Na-ion electrochemistry in layered bismuth telluride anodes

Abstract

Van der Waals layered metal chalcogenide Bi2Te3 has shown exceptional capacity and rate capability in alkali-ion batteries but the underlying reaction mechanism with Li+, Na+, and K+ remains undiscovered. It is unexpected that Na+ electrochemistry outperforms Li+ and K+ at high current densities. Here, in situ transmission electron microscopy is used to uncover nanoscale transformations during lithiation, sodiation, and potassiation, which follows two-step conversion and alloying reactions with Li+ and Na+, and three-step intercalation-conversion-alloying reactions with K+. Counterintuitively, sodiation exhibits the highest reaction kinetics, and its origin can be elucidated by first-principles and finite-element simulations in two aspects. The lower interfacial strain accommodation energy between Bi2Te3 and its Na-conversion products allows more facile sodiation phase transformation than Li- and K-ion reactions. The higher chemo-mechanical stress concentration at the concave-shaped sodiation reaction front facilitates continued Na-ion diffusion and reaction propagation. These fundamental insights are essential for fast-charging alkali-ions batteries.

Authors:
ORCiD logo; ; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
OSTI Identifier:
1763837
Alternate Identifier(s):
OSTI ID: 1764009; OSTI ID: 1764591
Report Number(s):
BNL-220971-2021-JAAM; BNL-220984-2021-JAAM
Journal ID: ISSN 2590-2385; S2590238521000059; PII: S2590238521000059
Grant/Contract Number:  
SC0012704
Resource Type:
Published Article
Journal Name:
Matter (Online)
Additional Journal Information:
Journal Name: Matter (Online); Journal ID: ISSN 2590-2385
Publisher:
Cell Press/Elsevier
Country of Publication:
United States
Language:
English
Subject:
29 ENERGY PLANNING, POLICY, AND ECONOMY; 25 ENERGY STORAGE; Li-ion batteries; Na-ion batteries; K-ion batteries; in situ TEM; Bi2Te3; metal chalcogenides; chemo-mechanical stress; reaction front geometry; electrochemo-mechanical stress; sodiation; potassiation

Citation Formats

Cui, Jiang, Zheng, Hongkui, Zhang, Zilong, Hwang, Sooyeon, Yang, Xiao-Qing, and He, Kai. Origin of anomalous high-rate Na-ion electrochemistry in layered bismuth telluride anodes. United States: N. p., 2021. Web. doi:10.1016/j.matt.2021.01.005.
Cui, Jiang, Zheng, Hongkui, Zhang, Zilong, Hwang, Sooyeon, Yang, Xiao-Qing, & He, Kai. Origin of anomalous high-rate Na-ion electrochemistry in layered bismuth telluride anodes. United States. https://doi.org/10.1016/j.matt.2021.01.005
Cui, Jiang, Zheng, Hongkui, Zhang, Zilong, Hwang, Sooyeon, Yang, Xiao-Qing, and He, Kai. Mon . "Origin of anomalous high-rate Na-ion electrochemistry in layered bismuth telluride anodes". United States. https://doi.org/10.1016/j.matt.2021.01.005.
@article{osti_1763837,
title = {Origin of anomalous high-rate Na-ion electrochemistry in layered bismuth telluride anodes},
author = {Cui, Jiang and Zheng, Hongkui and Zhang, Zilong and Hwang, Sooyeon and Yang, Xiao-Qing and He, Kai},
abstractNote = {Van der Waals layered metal chalcogenide Bi2Te3 has shown exceptional capacity and rate capability in alkali-ion batteries but the underlying reaction mechanism with Li+, Na+, and K+ remains undiscovered. It is unexpected that Na+ electrochemistry outperforms Li+ and K+ at high current densities. Here, in situ transmission electron microscopy is used to uncover nanoscale transformations during lithiation, sodiation, and potassiation, which follows two-step conversion and alloying reactions with Li+ and Na+, and three-step intercalation-conversion-alloying reactions with K+. Counterintuitively, sodiation exhibits the highest reaction kinetics, and its origin can be elucidated by first-principles and finite-element simulations in two aspects. The lower interfacial strain accommodation energy between Bi2Te3 and its Na-conversion products allows more facile sodiation phase transformation than Li- and K-ion reactions. The higher chemo-mechanical stress concentration at the concave-shaped sodiation reaction front facilitates continued Na-ion diffusion and reaction propagation. These fundamental insights are essential for fast-charging alkali-ions batteries.},
doi = {10.1016/j.matt.2021.01.005},
journal = {Matter (Online)},
number = ,
volume = ,
place = {United States},
year = {Mon Feb 01 00:00:00 EST 2021},
month = {Mon Feb 01 00:00:00 EST 2021}
}

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