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Operando Electrochemical Liquid-Cell Scanning Transmission Electron Microscopy (EC-STEM) Studies of Evolving Cu Nanocatalysts for CO2 Electroreduction

Journal Article · · ACS Sustainable Chemistry & Engineering
 [1];  [2];  [3];  [1];  [1];  [1];  [4];  [1];  [1];  [2];  [2];  [5]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  2. Cornell Univ., Ithaca, NY (United States)
  3. Univ. of California, Berkeley, CA (United States)
  4. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  5. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)
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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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); National Science Foundation (NSF)
Grant/Contract Number:
AC02-05CH11231; SC0019445
OSTI ID:
2229312
Journal Information:
ACS Sustainable Chemistry & Engineering, Journal Name: ACS Sustainable Chemistry & Engineering Journal Issue: 10 Vol. 11; ISSN 2168-0485
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
4D-STEM
CO2RR
EC-STEM
cu nanocatalysts
dynamic evolution
operando