Crystallographically vacancy‐induced MOF nanosheet as rational single‐atom support for accelerating CO2 electroreduction to COopen access
- Authors
- Cho, Jin Hyuk; Ma, Joonhee; Lee, Chaehyeon; Lim, Jin Wook; Kim, Youngho; Jang, Ho Yeon; Kim, Jaehyun; Seo, Myung-gi; Choi, Youngheon; Jang, Youn Jeong; Ahn, Sang Hyun; Jang, Ho Won; Back, Seoin; Lee, Jong-Lam; Kim, Soo Young
- Issue Date
- Feb-2024
- Publisher
- WILEY
- Keywords
- 2-dimensional material; carbon dioxide reduction; metal-organic frameworks; single-atom catalysts; vacancy sites
- Citation
- CARBON ENERGY
- Journal Title
- CARBON ENERGY
- URI
- https://scholarworks.bwise.kr/cau/handle/2019.sw.cau/73027
- DOI
- 10.1002/cey2.510
- ISSN
- 2637-9368
2637-9368
- Abstract
- To attain a circular carbon economy and resolve CO2 electroreduction technology obstacles, single-atom catalysts (SACs) have emerged as a logical option for electrocatalysis because of their extraordinary catalytic activity. Among SACs, metal-organic frameworks (MOFs) have been recognized as promising support materials because of their exceptional ability to prevent metal aggregation. This study shows that atomically dispersed Ni single atoms on a precisely engineered MOF nanosheet display a high Faradaic efficiency of approximately 100% for CO formation in H-cell and three-compartment microfluidic flow-cell reactors and an excellent turnover frequency of 23,699 h(-1), validating their intrinsic catalytic potential. These results suggest that crystallographic variations affect the abundant vacancy sites on the MOF nanosheets, which are linked to the evaporation of Zn-containing organic linkers during pyrolysis. Furthermore, using X-ray absorption spectroscopy and density functional theory calculations, a comprehensive investigation of the unsaturated atomic coordination environments and the underlying mechanism involving CO* preadsorbed sites as initial states was possible and provided valuable insights.
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