Citation: Xiang-Da Zhang, Jian-Mei Huang, Xiaorong Zhu, Chang Liu, Yue Yin, Jia-Yi Huang, Yafei Li, Zhi-Yuan Gu. Auto-tandem CO₂ reduction by reconstructed Cu imidazole framework isomers: Unveiling pristine MOF-mediated CO₂ activation[J]. Chinese Chemical Letters, ;2025, 36(5): 109937. doi: 10.1016/j.cclet.2024.109937 shu

Auto-tandem CO₂ reduction by reconstructed Cu imidazole framework isomers: Unveiling pristine MOF-mediated CO₂ activation

Xiang-Da Zhang ^{a, 1} ,
Jian-Mei Huang ^{a, 1} ,
Xiaorong Zhu ^{b, 1} ,
Chang Liu ^a ,
Yue Yin ^a ,
Jia-Yi Huang ^a ,
Yafei Li ^{a, *,} ,
Zhi-Yuan Gu ^{a, *,}

a.
Jiangsu Key Laboratory of Biofunctional Materials, Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, College of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, China
b.
School of Chemistry and Chemical Engineering, Nantong University, Nantong 226019, China

yafeili@njnu.edu.cn

guzhiyuan@njnu.edu.cn

Received Date: 8 March 2024
Revised Date: 2 April 2024
Accepted Date: 28 April 2024
Available Online: 29 April 2024

Figures(5)

Cu-based metal-organic frameworks (MOFs) are widely employed in CO₂ reduction reactions (CO₂RR). Mostly, the in-situ reconstructed derivatives such as Cu or Cu oxides during CO₂RR are regarded as the catalytic active center for the formation of catalytic products. However, in many cases, the pristine MOFs still exist during the catalytic process, the key role of these pristine MOFs is often ignored in revealing the catalytic mechanism. Here, we designed two Cu(imidazole) with different coordination environments, namely CuN₂ and Cu₂N₄ for CO₂RR. The structures of the two MOFs were still remained after the catalytic reaction. We discovered that the pristine MOFs served as activation catalysts for converting CO₂ into CO. Sequentially, the Cu-based derivatives, in the two cases, Cu(111) converted the CO into C₂₊ products. The CuN₂ with more exposed Cu-N centers showed a higher FE_CO and a higher final FE_C2+ than Cu₂N₄. This auto-tandem catalytic mechanism was supported by electrocatalytic performance, TPD-CO, HRTEM, SAED, XPS, in-situ XANES and XES and DFT computation. The auto-tandem catalytic mechanism provides a new route to design Cu-based MOF electrocatalysts for high product selectivity in CO₂RR.
- CO₂ reduction reactions,
- Cu-based MOF,
- In-situ reconstructed,
- Coordination environment,
- Auto-tandem catalysis
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Auto-tandem CO2 reduction by reconstructed Cu imidazole framework isomers: Unveiling pristine MOF-mediated CO2 activation

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通讯作者: 陈斌, bchen63@163.com

Auto-tandem CO₂ reduction by reconstructed Cu imidazole framework isomers: Unveiling pristine MOF-mediated CO₂ activation