Mixed-valence Cu-based metal-organic framework for selective CO_(2) electroreduction to C_(1) liquid fuels with high energy conversion efficiency  

作　　者：Luyao Wang Fengting Li Yifan Gu 

机构地区：[1]College of Environmental Science and Engineering,State Key Laboratory of Pollution Control and Resource Reuse,Tongji University,Shanghai 200092,China [2]Shanghai Institute of Pollution Control and Ecological Security,Shanghai 200092,China [3]Key Laboratory of Cities’Mitigation and Adaptation to Climate Change,Shanghai,China Meteorological Administration(CMA),Tongji University,Shanghai 200092,China

出　　处：《Nano Research》2025年第4期153-160,共8页纳米研究(英文版)

基　　金：granted by the National Natural Science Foundation of China(Nos.22376161 and 52373216);the National Key Research and Development Program of China(No.2022YFE0110500);the Fundamental Research Funds for the Central Universities of China.

摘　　要：Efficient CO_(2) electroreduction requires catalysts for enhanced energy conversion efficiency and carbon product selectivity with low overpotential,in consideration of the interference of competitive H_(2) 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 CO_(2).The designed material delivered a remarkable Faradaic efficiency of 99.2%for C_(1) 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 CO_(2) conversion.

关 键 词：metal-organic frameworks CO_(2)electroreduction MIXED-VALENCE energy conversion efficiency liquid fuels CATALYSIS 

分 类 号：O643.36[理学—物理化学]