Precisely Constructing Orbital Coupling-Modulated Dual-Atom Fe Pair Sites for Synergistic CO2 Electroreduction
SCIE
SCOPUS
- Title
- Precisely Constructing Orbital Coupling-Modulated Dual-Atom Fe Pair Sites for Synergistic CO2 Electroreduction
- Authors
- Wang, Ying; Park, Byoung Joon; Paidi, Vinod K.; Huang, Rui; Lee, Yechan; Noh, Kyung-Jong; Lee, Kug-Seung; Han, Jeong Woo
- Date Issued
- 2022-02-11
- Publisher
- AMER CHEMICAL SOC
- Abstract
- Electrochemical reduction of CO2 (CO2RR) provides an attractive pathway to achieve a carbon-neutral energy cycle. Single-atom catalysts (SAC) have shown unique potential in heterogeneous catalysis, but their structural simplicity prevents them from breaking linear scaling relationships. In this study, we develop a feasible strategy to precisely construct a series of electrocatalysts featuring well-defined single-atom and dual-site iron anchored on nitrogen-doped carbon matrix (Fe1–N–C and Fe2–N–C). The Fe2–N–C dual-atom electrocatalyst (DAC) achieves enhanced CO Faradaic efficiency above 80% in wider applied potential ranges along with higher turnover frequency (26,637 h–1) and better durability compared to SAC counterparts. Furthermore, based on in-depth experimental and theoretical analysis, the orbital coupling between the iron dual sites decreases the energy gap between antibonding and bonding states in *CO adsorption. This research presents new insights into the structure–performance relationship on CO2RR electrocatalysts at the atomic scale and extends the application of DACs for heterogeneous electrocatalysis and beyond.
- URI
- https://oasis.postech.ac.kr/handle/2014.oak/109310
- DOI
- 10.1021/acsenergylett.1c02446
- ISSN
- 2380-8195
- Article Type
- Article
- Citation
- Acs Energy Letters, vol. 7, no. 2, page. 640 - 649, 2022-02-11
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