Emerging Electrochemical Techniques for Probing Site Behavior in Single-Atom Electrocatalysts
Abstract
Single-atom catalysts (SACs) have aroused tremendous interest over the past decade, particularly in the community of energy and environment-related electrocatalysis. A rapidly growing number of recent publications have recognized it as a promising candidate with maximum atomic utilization, distinct activity, and selectivity in comparison to bulk catalysts and nanocatalysts. However, the complexity of localized coordination environments and the dispersion of isolated sites lead to significant difficulties when it comes to gaining insight into the intrinsic behavior of electrocatalytic reactions. Furthermore, the low metal loadings of most SACs make conventional ensemble measurements less likely to be accurate on the subnanoscale. Thus, it remains challenging to probe the activity and properties of individual atomic sites by available commercial instruments and analytical methods. In spite of this, continuing efforts have lately focused on the development of advanced measurement methodologies, which are very useful to the fundamental understanding of SACs. There have recently been a number of in situ/operando techniques applied to SACs, such as electron microscopy, spectroscopy, and other analysis methods, which support relevant functions to identify the active sites and reaction intermediates and to investigate the dynamic behavior of localized structures of the catalytic sites. This Account aims to present recent electrochemicalmore »
- Authors:
-
- University of Electronic Science and Technology of China, Chengdu (P. R. China)
- Univ. of Texas, Austin, TX (United States); University of Electronic Science and Technology of China, Chengdu (P. R. China)
- Univ. of Texas, Austin, TX (United States)
- Publication Date:
- Research Org.:
- Univ. of Texas, Austin, TX (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Welch Foundation
- OSTI Identifier:
- 1865381
- Grant/Contract Number:
- SC0019019; F-1861
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Accounts of Chemical Research
- Additional Journal Information:
- Journal Volume: 55; Journal Issue: 5; Journal ID: ISSN 0001-4842
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Anions; Probes; Kinetics; Redox reactions; Catalysts
Citation Formats
Jin, Zhaoyu, Li, Panpan, Fang, Zhiwei, and Yu, Guihua. Emerging Electrochemical Techniques for Probing Site Behavior in Single-Atom Electrocatalysts. United States: N. p., 2022.
Web. doi:10.1021/acs.accounts.1c00785.
Jin, Zhaoyu, Li, Panpan, Fang, Zhiwei, & Yu, Guihua. Emerging Electrochemical Techniques for Probing Site Behavior in Single-Atom Electrocatalysts. United States. https://doi.org/10.1021/acs.accounts.1c00785
Jin, Zhaoyu, Li, Panpan, Fang, Zhiwei, and Yu, Guihua. Fri .
"Emerging Electrochemical Techniques for Probing Site Behavior in Single-Atom Electrocatalysts". United States. https://doi.org/10.1021/acs.accounts.1c00785. https://www.osti.gov/servlets/purl/1865381.
@article{osti_1865381,
title = {Emerging Electrochemical Techniques for Probing Site Behavior in Single-Atom Electrocatalysts},
author = {Jin, Zhaoyu and Li, Panpan and Fang, Zhiwei and Yu, Guihua},
abstractNote = {Single-atom catalysts (SACs) have aroused tremendous interest over the past decade, particularly in the community of energy and environment-related electrocatalysis. A rapidly growing number of recent publications have recognized it as a promising candidate with maximum atomic utilization, distinct activity, and selectivity in comparison to bulk catalysts and nanocatalysts. However, the complexity of localized coordination environments and the dispersion of isolated sites lead to significant difficulties when it comes to gaining insight into the intrinsic behavior of electrocatalytic reactions. Furthermore, the low metal loadings of most SACs make conventional ensemble measurements less likely to be accurate on the subnanoscale. Thus, it remains challenging to probe the activity and properties of individual atomic sites by available commercial instruments and analytical methods. In spite of this, continuing efforts have lately focused on the development of advanced measurement methodologies, which are very useful to the fundamental understanding of SACs. There have recently been a number of in situ/operando techniques applied to SACs, such as electron microscopy, spectroscopy, and other analysis methods, which support relevant functions to identify the active sites and reaction intermediates and to investigate the dynamic behavior of localized structures of the catalytic sites. This Account aims to present recent electrochemical probing techniques which can be used to identify single-atomic catalytic sites within solid supports. First, we describe the basic principles of molecular probe methods for the study and analysis of electrocatalytic site behavior. In particular, the in situ probing technique enabled by surface interrogation scanning electrochemical microscopy (SISECM) can measure the active site density and kinetic rate with high resolution. An alternative electrochemical probing technique is further demonstrated on the basis of single-entity electrochemistry, which allows the unique electrochemical imaging of the size and catalytic rate of single atoms, molecules, and clusters. Next, the merits and limitations of different electrochemical techniques are then discussed, along with perspectives for future prospects. Apart from this, we further showcase the powerful capability of emerging electrochemical probing techniques for determining significant effects and properties of SACs for various electrocatalytic reactions, including oxygen reduction and evolution, hydrogen evolution, and nitrate reduction. Overall, electrochemical techniques with atomic resolution have greatly increased opportunities for observing, measuring, and understanding the surface and interface chemistry during energy conversion. In the future, it is anticipated that the development of electrochemical probing techniques will be advanced with innovative perspectives on the behavior and features of SACs. We hope that this Account can contribute in several ways to promoting the fundamental knowledge and technical progress of emerging electrochemical measurements for studying SACs.},
doi = {10.1021/acs.accounts.1c00785},
journal = {Accounts of Chemical Research},
number = 5,
volume = 55,
place = {United States},
year = {Fri Feb 11 00:00:00 EST 2022},
month = {Fri Feb 11 00:00:00 EST 2022}
}
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