Transition Metal Ion Doping on ZIF-8 Enhances the Electrochemical CO2 Reduction Reaction
- Authors
- Cho, Jin Hyuk; Lee, Chaehyeon; Hong, Sung Hyun; Jang, Ho Yeon; Back, Seoin; Seo, Myung-gi; Jang, Youn Jeong; Ahn, Sang Hyun; Jang, Ho Won; Kim, Soo Young; Choi, Youngheon; Lee, Minzae; Min, Hyung-Ki
- Issue Date
- Oct-2023
- Publisher
- WILEY-V C H VERLAG GMBH
- Keywords
- carbon dioxide reduction; carbon monoxide; electrocatalyst; local effects; sp(2) C; ZIF-8
- Citation
- ADVANCED MATERIALS, v.35, no.43, pp.1 - 9
- Indexed
- SCIE
SCOPUS
- Journal Title
- ADVANCED MATERIALS
- Volume
- 35
- Number
- 43
- Start Page
- 1
- End Page
- 9
- URI
- https://scholarworks.bwise.kr/hanyang/handle/2021.sw.hanyang/192865
- DOI
- 10.1002/adma.202208224
- ISSN
- 0935-9648
- Abstract
- The electrochemical reduction of CO2 to diverse value-added chemicals is a unique, environmentally friendly approach for curbing greenhouse gas emissions while addressing sluggish catalytic activity and low Faradaic efficiency (FE) of electrocatalysts. Here, zeolite-imidazolate-frameworks-8 (ZIF-8) containing various transition metal ions-Ni, Fe, and Cu-at varying concentrations upon doping are fabricated for the electrocatalytic CO2 reduction reaction (CO2RR) to carbon monoxide (CO) without further processing. Atom coordination environments and theoretical electrocatalytic performance are scrutinized via X-ray absorption spectroscopy (XAS) and density functional theory (DFT) calculations. Upon optimized Cu doping on ZIF-8, Cu0.5Zn0.5/ZIF-8 achieves a high partial current density of 11.57 mA cm(-2) and maximum FE for CO of 88.5% at -1.0 V (versus RHE) with a stable catalytic activity over 6 h. Furthermore, the electron-rich sp(2) C atom facilitates COOH* promotion after Cu doping of ZIF-8, leading to a local effect between the zinc-nitrogen (Zn-N-4) and copper-nitrogen (Cu-N-4) moieties. Additionally, the advanced CO2RR pathway is illustrated from various perspectives, including the pre-H-covered state under the CO2RR. The findings expand the pool of efficient metal-organic framework (MOF)-based CO2RR catalysts, deeming them viable alternatives to conventional catalysts.
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