Design principles for heterointerfacial alloying kinetics at metallic anodes in rechargeable batteries

Zheng, Jingxu; Deng, Yue; Li, Wenzao; Yin, Jiefu; West, Patrick J.; Tang, Tian; Tong, Xiao; Bock, David C.; Jin, Shuo; Zhao, Qing; Garcia-Mendez, Regina; Takeuchi, Kenneth J.; Takeuchi, Esther S.; Marschilok, Amy C.; Archer, Lynden A.

doi:10.1126/sciadv.abq6321

Design principles for heterointerfacial alloying kinetics at metallic anodes in rechargeable batteries

Journal Article · Fri Nov 04 00:00:00 EDT 2022 · Science Advances

DOI:https://doi.org/10.1126/sciadv.abq6321· OSTI ID:2420258

^[1]; ^[2]; ^[3]; Yin, Jiefu ^[2]; ^[4]; ^[2]; ^[5]; ^[6]; ^[2]; ^[2]; ^[2]; ^[7]; ^[7]; ^[7]; ^[2]

Cornell Univ., Ithaca, NY (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Cornell Univ., Ithaca, NY (United States)
Cornell Univ., Ithaca, NY (United States)
State Univ. of New York (SUNY), Stony Brook, NY (United States); Stony Brook Univ., NY (United States)
Stony Brook Univ., NY (United States); State Univ. of New York (SUNY), Stony Brook, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
State Univ. of New York (SUNY), Stony Brook, NY (United States); Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

How surface chemistry influences reactions occurring thereupon has been a long-standing question of broad scientific and technological interest. Here, we consider the relation between the surface chemistry at interfaces and the reversibility of electrochemical transformations at rechargeable battery electrodes. Using Zn as a model system, we report that a moderate strength of chemical interaction between the deposit and the substrate—neither too weak nor too strong—enables highest reversibility and stability of the plating/stripping redox processes. Focused ion beam and electron microscopy were used to directly probe the morphology, chemistry, and crystallography of heterointerfaces of distinct natures. Analogous to the empirical Sabatier principle for chemical heterogeneous catalysis, our findings arise from competing interfacial processes. Using full batteries with stringent negative electrode–to–positive electrode capacity (N:P) ratios, we show that such knowledge provides a powerful tool for designing key materials in highly reversible battery systems based on Earth-abundant, low-cost metals such as Zn and Na.

View Accepted Manuscript (DOE)

Research Organization:: State Univ. of New York (SUNY), Albany, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0012673

OSTI ID:: 2420258

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 44 Vol. 8; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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