Operando Heating and Cooling Electrochemical 4D-STEM Probing Nanoscale Dynamics at Solid–Liquid InterfacesClick to copy article linkArticle link copied!
- Sungin KimSungin KimDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Sungin Kim
- Valentin Briega-MartosValentin Briega-MartosDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Valentin Briega-Martos
- Shikai LiuShikai LiuDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Shikai Liu
- Kwanghwi JeKwanghwi JeDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Kwanghwi Je
- Chuqiao ShiChuqiao ShiDepartment of Materials Science and Nano Engineering, Rice University, Houston, Texas 77005, United StatesMore by Chuqiao Shi
- Katherine Marusak StephensKatherine Marusak StephensProtochips Inc., Morrisville, North Carolina 27560, United StatesMore by Katherine Marusak Stephens
- Steven E. ZeltmannSteven E. ZeltmannPlatform for the Accelerated Realization, Analysis, and Discovery of Interface Materials, Cornell University, Ithaca, New York 14853, United StatesMore by Steven E. Zeltmann
- Zhijing ZhangZhijing ZhangDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Zhijing Zhang
- Rafael Guzman-SorianoRafael Guzman-SorianoDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Rafael Guzman-Soriano
- Wenqi LiWenqi LiDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Wenqi Li
- Jiahong JiangJiahong JiangDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Jiahong Jiang
- Juhyung ChoiJuhyung ChoiDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Juhyung Choi
- Yafet J. NegashYafet J. NegashDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Yafet J. Negash
- Franklin S. Walden IIFranklin S. Walden, IIProtochips Inc., Morrisville, North Carolina 27560, United StatesMore by Franklin S. Walden, II
- Nelson L. Marthe Jr.Nelson L. Marthe, Jr.Protochips Inc., Morrisville, North Carolina 27560, United StatesMore by Nelson L. Marthe, Jr.
- Patrick S. WellbornPatrick S. WellbornProtochips Inc., Morrisville, North Carolina 27560, United StatesMore by Patrick S. Wellborn
- Yaofeng Guo
- John Damiano
- Yimo HanYimo HanDepartment of Materials Science and Nano Engineering, Rice University, Houston, Texas 77005, United StatesMore by Yimo Han
- Erik H. ThiedeErik H. ThiedeDepartment of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesMore by Erik H. Thiede
- Yao Yang*Yao Yang*Email: [email protected]Department of Chemistry and Chemical Biology, Baker Lab, Cornell University, Ithaca, New York 14853, United StatesKavli Institute at Cornell for Nanoscale Science, Cornell University, Ithaca, New York 14853, United StatesMore by Yao Yang
Abstract
Operando/in situ methods have revolutionized our fundamental understanding of molecular and structural changes at solid–liquid interfaces and enabled the vision of “watching chemistry in action”. Operando transmission electron microscopy (TEM) emerges as a powerful tool to interrogate time-resolved nanoscale dynamics, which involve local electrical fields and charge transfer kinetics distinctly different from those of their bulk counterparts. Despite early reports on electrochemical or heating liquid-cell TEM, developing operando TEM with simultaneous electrochemical and thermal control remains a formidable challenge. Here, we developed operando heating and cooling electrochemical liquid-cell scanning TEM (EC-STEM). By integrating a three-electrode electrochemical circuit and an additional two-electrode thermal circuit, we can investigate heterogeneous electrochemical kinetics across a wide temperature range of −50 to 300 °C. We used Cu electrodeposition/stripping processes as a model system to demonstrate quantitative electrochemistry from −40 to 95 °C in both transient and steady states in aqueous and organic solutions, which paves the way for investigating energy materials operating in extreme climates. Machine learning-assisted quantitative 4D-STEM structural analysis in cold liquids (−40 °C) reveals a distinct two-stage growth of nanometer-scale mossy Cu nanoislands with random orientations followed by μm-scale Cu dendrites with preferential orientations. This work benchmarked electrochemistry in the three-electrode EC-STEM and systematically investigated the temperature and pH dependence of the Pt pseudoreference electrode (RE). At room temperature, the Pt pseudo-RE shows a reliable potential of 0.8 ± 0.1 V vs the standard hydrogen electrode and remains pH-independent on the reversible hydrogen electrode scale. We anticipate that operando heating/cooling EC-STEM will become invaluable for understanding fundamental temperature-controlled nanoscale electrochemistry and advancing renewable energy technologies (e.g., catalysts and batteries) in realistic climates.
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