The influence of pressure on lithium dealloying in solid-state and liquid electrolyte batteries

IF 37.2 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Congcheng Wang, Yuhgene Liu, Won Joon Jeong, Timothy Chen, Mu Lu, Douglas Lars Nelson, Elif Pınar Alsaç, Sun Geun Yoon, Kelsey Anne Cavallaro, Sazol Das, Diptarka Majumdar, Rajesh Gopalaswamy, Shuman Xia, Matthew T. McDowell
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Abstract

Dealloying reactions underpin the operation of next-generation battery electrodes and are also a synthesis route for porous metals, but the influence of mechanical stress on these processes is not well understood. Here we investigate how the applied stack pressure affects structural evolution and electrochemical reversibility during the alloying/dealloying of Li alloy materials (Li–Al, Li–Sn, Li–In and Li–Si) using solid-state and liquid electrolytes. The extent of porosity formation during the dealloying of metals is found to be universally governed by stack pressure, with pressures of at least 20% of the yield strength required to achieve ~80% relative density. This concept is correlated to the cycling of alloy electrodes in solid-state batteries, with a yield-strength-dependent threshold pressure needed for reversible high Li-storage capacity due to densification. With this understanding, we design Al and Si anodes with a densified interfacial layer enabling stable cycling at low stack pressures (2 MPa), providing guidance towards practical high-energy solid-state batteries.

Abstract Image

压力对固态和液态电解质电池中锂脱合金的影响
脱合金反应是下一代电池电极的基础,也是多孔金属的合成途径,但机械应力对这些过程的影响尚不清楚。在这里,我们研究了应用堆压如何影响锂合金材料(Li - al, Li - sn, Li - in和Li - si)在固态和液态电解质的合金化/脱合金过程中的结构演变和电化学可逆性。研究发现,金属合金化过程中孔隙形成的程度普遍受堆积压力的影响,要达到80%的相对密度,堆积压力至少要达到屈服强度的20%。这一概念与固态电池中合金电极的循环有关,由于致密化,需要屈服强度相关的阈值压力来实现可逆的高锂存储容量。基于这一认识,我们设计了具有致密界面层的Al和Si阳极,使其能够在低堆叠压力(2 MPa)下稳定循环,为实用的高能固态电池提供指导。
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来源期刊
Nature Materials
Nature Materials 工程技术-材料科学:综合
CiteScore
62.20
自引率
0.70%
发文量
221
审稿时长
3.2 months
期刊介绍: Nature Materials is a monthly multi-disciplinary journal aimed at bringing together cutting-edge research across the entire spectrum of materials science and engineering. It covers all applied and fundamental aspects of the synthesis/processing, structure/composition, properties, and performance of materials. The journal recognizes that materials research has an increasing impact on classical disciplines such as physics, chemistry, and biology. Additionally, Nature Materials provides a forum for the development of a common identity among materials scientists and encourages interdisciplinary collaboration. It takes an integrated and balanced approach to all areas of materials research, fostering the exchange of ideas between scientists involved in different disciplines. Nature Materials is an invaluable resource for scientists in academia and industry who are active in discovering and developing materials and materials-related concepts. It offers engaging and informative papers of exceptional significance and quality, with the aim of influencing the development of society in the future.
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