Journal
MATTER
Volume 4, Issue 4, Pages 1335-1351Publisher
CELL PRESS
DOI: 10.1016/j.matt.2021.01.005
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Funding
- Clemson University start-up fund
- National Science Foundation [1929138]
- US DOE Office of Science Facility, at Brookhaven National Laboratory [DE-SC0012704]
- Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technologies Office of the US Department of Energy through the Advanced Battery Materials Research (BMR) Program [DE-SC0012704]
- Office Of The Director
- Office of Integrative Activities [1929138] Funding Source: National Science Foundation
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In situ transmission electron microscopy was used to uncover nanoscale transformations during lithiation, sodiation, and potassiation of Bi2Te3 in alkali-ion batteries, with sodiation exhibiting the highest reaction kinetics. The origin of this phenomenon was elucidated through first-principles and finite-element simulations, pointing to lower interfacial strain accommodation energy and higher electrochemo-mechanical stress concentration as key factors. These insights are crucial for fast-charging alkali-ion batteries.
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 electrochemo-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-ion batteries.
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