Atomic dynamics of electrified solid–liquid interfaces in liquid-cell TEM

Qiubo Zhang, Zhigang Song, Xianhu Sun, Yang Liu, Jiawei Wan, Sophia B. Betzler, Qi Zheng, Junyi Shangguan, Karen C. Bustillo, Peter Ercius, Prineha Narang, Yu Huang and Haimei Zheng ()
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Qiubo Zhang: Lawrence Berkeley National Laboratory
Zhigang Song: Harvard University
Xianhu Sun: Lawrence Berkeley National Laboratory
Yang Liu: University of California, Los Angeles
Jiawei Wan: Lawrence Berkeley National Laboratory
Sophia B. Betzler: Lawrence Berkeley National Laboratory
Qi Zheng: Lawrence Berkeley National Laboratory
Junyi Shangguan: Lawrence Berkeley National Laboratory
Karen C. Bustillo: Lawrence Berkeley National Laboratory
Peter Ercius: Lawrence Berkeley National Laboratory
Prineha Narang: University of California, Los Angeles
Yu Huang: University of California, Los Angeles
Haimei Zheng: Lawrence Berkeley National Laboratory

Nature, 2024, vol. 630, issue 8017, 643-647

Abstract: Abstract Electrified solid–liquid interfaces (ESLIs) play a key role in various electrochemical processes relevant to energy1–5, biology6 and geochemistry7. The electron and mass transport at the electrified interfaces may result in structural modifications that markedly influence the reaction pathways. For example, electrocatalyst surface restructuring during reactions can substantially affect the catalysis mechanisms and reaction products1–3. Despite its importance, direct probing the atomic dynamics of solid–liquid interfaces under electric biasing is challenging owing to the nature of being buried in liquid electrolytes and the limited spatial resolution of current techniques for in situ imaging through liquids. Here, with our development of advanced polymer electrochemical liquid cells for transmission electron microscopy (TEM), we are able to directly monitor the atomic dynamics of ESLIs during copper (Cu)-catalysed CO2 electroreduction reactions (CO2ERs). Our observation reveals a fluctuating liquid-like amorphous interphase. It undergoes reversible crystalline–amorphous structural transformations and flows along the electrified Cu surface, thus mediating the crystalline Cu surface restructuring and mass loss through the interphase layer. The combination of real-time observation and theoretical calculations unveils an amorphization-mediated restructuring mechanism resulting from charge-activated surface reactions with the electrolyte. Our results open many opportunities to explore the atomic dynamics and its impact in broad systems involving ESLIs by taking advantage of the in situ imaging capability.

Date: 2024
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DOI: 10.1038/s41586-024-07479-w

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