Operando Electrochemical Liquid-Cell Scanning Transmission Electron Microscopy (EC-STEM) Studies of Evolving Cu Nanocatalysts for CO2 Electroreduction
Abstract
The design and synthesis of nanocatalysts with well-defined sizes, compositions, and structures have revolutionized our accessibility to tunable catalyst activity and selectivity for a variety of energy-related electrochemical reactions. Nonetheless, establishing structure-(re)activity correlations requires the understanding of the dynamic evolution of pristine nanocatalysts and the identification of their active states under operating conditions. We previously communicated the operando observation of Cu nanocatalysts evolving into active metallic Cu nanograins for CO2 electroreduction (Yang et al. Nature 2023, 614, 262–269). Here, we expand our discussion to the technical capabilities and further research applications of operando electrochemical liquid-cell scanning transmission electron microscopy (EC-STEM), which enables quantitative electrochemistry while tracking dynamic structural evolution of sub-10 nm Cu nanocatalysts. The coexistent H2 bubbles, often disruptive to operando spectroscopy, are an effective approach to create a thin-liquid layer that significantly improves spatial resolution while remaining electrochemically accessible to Cu nanocatalysts. Operando four-dimensional (4D) STEM in liquids provides insights into the complex structure of active polycrystalline metallic Cu nanograins. With continuous technical developments, we anticipate that operando EC-STEM will evolve into a powerful electroanalytical method to advance our understanding of a variety of nanoscale electrocatalysts at solid/liquid interfaces.
- Authors:
-
[1];
[3];
[1];
[1];
[4];
[1];
[2];
[2];
[5]
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Cornell Univ., Ithaca, NY (United States)
- Univ. of California, Berkeley, CA (United States)
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF)
- OSTI Identifier:
- 2229312
- Grant/Contract Number:
- AC02-05CH11231; SC0019445; DMR-1719875
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Sustainable Chemistry & Engineering
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 10; Journal ID: ISSN 2168-0485
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; operando; EC-STEM; 4D-STEM; CO2RR; dynamic evolution; cu nanocatalysts
Citation Formats
Yang, Yao, Shao, Yu-Tsun, Jin, Jianbo, Feijóo, Julian, Roh, Inwhan, Louisia, Sheena, Yu, Sunmoon, Fonseca Guzman, Maria V., Chen, Chubai, Muller, David A., Abruña, Héctor D., and Yang, Peidong. Operando Electrochemical Liquid-Cell Scanning Transmission Electron Microscopy (EC-STEM) Studies of Evolving Cu Nanocatalysts for CO2 Electroreduction. United States: N. p., 2023.
Web. doi:10.1021/acssuschemeng.2c06542.
Yang, Yao, Shao, Yu-Tsun, Jin, Jianbo, Feijóo, Julian, Roh, Inwhan, Louisia, Sheena, Yu, Sunmoon, Fonseca Guzman, Maria V., Chen, Chubai, Muller, David A., Abruña, Héctor D., & Yang, Peidong. Operando Electrochemical Liquid-Cell Scanning Transmission Electron Microscopy (EC-STEM) Studies of Evolving Cu Nanocatalysts for CO2 Electroreduction. United States. https://doi.org/10.1021/acssuschemeng.2c06542
Yang, Yao, Shao, Yu-Tsun, Jin, Jianbo, Feijóo, Julian, Roh, Inwhan, Louisia, Sheena, Yu, Sunmoon, Fonseca Guzman, Maria V., Chen, Chubai, Muller, David A., Abruña, Héctor D., and Yang, Peidong. Sat .
"Operando Electrochemical Liquid-Cell Scanning Transmission Electron Microscopy (EC-STEM) Studies of Evolving Cu Nanocatalysts for CO2 Electroreduction". United States. https://doi.org/10.1021/acssuschemeng.2c06542. https://www.osti.gov/servlets/purl/2229312.
@article{osti_2229312,
title = {Operando Electrochemical Liquid-Cell Scanning Transmission Electron Microscopy (EC-STEM) Studies of Evolving Cu Nanocatalysts for CO2 Electroreduction},
author = {Yang, Yao and Shao, Yu-Tsun and Jin, Jianbo and Feijóo, Julian and Roh, Inwhan and Louisia, Sheena and Yu, Sunmoon and Fonseca Guzman, Maria V. and Chen, Chubai and Muller, David A. and Abruña, Héctor D. and Yang, Peidong},
abstractNote = {The design and synthesis of nanocatalysts with well-defined sizes, compositions, and structures have revolutionized our accessibility to tunable catalyst activity and selectivity for a variety of energy-related electrochemical reactions. Nonetheless, establishing structure-(re)activity correlations requires the understanding of the dynamic evolution of pristine nanocatalysts and the identification of their active states under operating conditions. We previously communicated the operando observation of Cu nanocatalysts evolving into active metallic Cu nanograins for CO2 electroreduction (Yang et al. Nature 2023, 614, 262–269). Here, we expand our discussion to the technical capabilities and further research applications of operando electrochemical liquid-cell scanning transmission electron microscopy (EC-STEM), which enables quantitative electrochemistry while tracking dynamic structural evolution of sub-10 nm Cu nanocatalysts. The coexistent H2 bubbles, often disruptive to operando spectroscopy, are an effective approach to create a thin-liquid layer that significantly improves spatial resolution while remaining electrochemically accessible to Cu nanocatalysts. Operando four-dimensional (4D) STEM in liquids provides insights into the complex structure of active polycrystalline metallic Cu nanograins. With continuous technical developments, we anticipate that operando EC-STEM will evolve into a powerful electroanalytical method to advance our understanding of a variety of nanoscale electrocatalysts at solid/liquid interfaces.},
doi = {10.1021/acssuschemeng.2c06542},
journal = {ACS Sustainable Chemistry & Engineering},
number = 10,
volume = 11,
place = {United States},
year = {Sat Feb 25 00:00:00 EST 2023},
month = {Sat Feb 25 00:00:00 EST 2023}
}
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