Mixed-valence Cu-based metal-organic framework for selective CO2 electroreduction to C1 liquid fuels with high energy conversion efficiency

被引:0
作者
Wang, Luyao [1 ]
Li, Fengting [1 ,2 ,3 ]
Gu, Yifan [1 ,2 ,3 ]
机构
[1] Tongji Univ, Coll Environm Sci & Engn, State Key Lab Pollut Control & Resource Reuse, Shanghai 200092, Peoples R China
[2] Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China
[3] Tongji Univ, Key Lab Cities Mitigat & Adaptat Climate Change, China Meteorol Adm CMA, Shanghai 200092, Peoples R China
基金
中国国家自然科学基金;
关键词
metal-organic frameworks; CO; 2; electroreduction; mixed-valence; energy conversion efficiency; liquid fuels; catalysis; REDUCTION; INTERFACE;
D O I
10.26599/NR.2025.94907317
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Efficient CO2 electroreduction requires catalysts for enhanced energy conversion efficiency and carbon product selectivity with low overpotential, in consideration of the interference of competitive H2 evolution reaction and complex intermediate species involved. We proposed that adaptive electronic structures based on dynamic mixed-valence interconversion would facilitate electron transfer and intermediate turnover during the catalysis, ensuring high activity, selectivity, and durability. Herein, a novel mixed-valence Cu-based metal-organic framework was prepared using an electron-rich linker for electrocatalytic reduction of CO2. The designed material delivered a remarkable Faradaic efficiency of 99.2% for C1 liquid fuels at a low reduction potential of -0.1 V versus reversible hydrogen electrode, considerably higher than that of the commercial copper foam and competitive to the Cu-based electrocatalysts reported. The experimental data and theoretical calculations verified the Cu(I)/Cu(II) interconversion and the much higher energy barrier of H2 evolution than carbon product generation. Such a feasible strategy, simultaneously improving energy conversion efficiency, carbon product selectivity, and structural robustness, provides great insights into rational catalyst customization for sustainable CO2 conversion.
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页数:8
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