室温快速合成Ag基金属有机骨架材料用于电催化还原CO2
Rapid synthesis of Ag-based metal-organic framework at room temperature for efficient electrocatalytic CO2 reduction
作者单位E-mail
车钰灿 武汉大学化学与分子科学学院, 武汉 430072  
程鹏玮 武汉大学化学与分子科学学院, 武汉 430072  
周毅 武汉大学化学与分子科学学院, 武汉 430072  
柯福生 武汉大学化学与分子科学学院, 武汉 430072 kefs@whu.edu.cn 
摘要: 选择具有强给电子能力的1,2,4-三唑为配体,成功合成了银基金属有机骨架材料(Ag-MOF)并用于电催化还原CO2反应(CO2RR)。借助粉末X射线衍射、透射电子显微镜、扫描电子显微镜、计时电流法等表征手段对材料的晶体结构、形貌和电催化CO2RR性能进行了系统的研究。与商品化的纳米Ag颗粒对比,Ag-MOF展现出更优异的电催化CO2RR产物选择性、催化活性和稳定性,在-0.9 V (vs RHE)时,CO的法拉第效率高达96.1%。当电压为-1.1 V (vs RHE)时,电流密度可达17 mA·cm-2,且电极可以稳定运行300 min。这说明通过选择合适的配体结构,可以改变催化位点周围的化学环境,从而高效将CO2转化为目标产物。
关键词: 金属有机骨架  银基金属有机骨架  电催化还原CO2  CO
基金项目: 国家自然科学基金(No.22172116,21773176)资助。
Abstract: An Ag-based metal-organic framework (Ag-MOF) material was successfully synthesized and used for the first time in the electrocatalytic CO2 reduction reaction (CO2RR) by selecting 1,2,4-triazole as the ligand with strong electron-donating ability. The crystal structure, morphology, and electrocatalytic CO2RR performance of Ag-MOF were systematically investigated using characterization methods such as powder X-ray diffraction, transmission electron microscopy, scanning electron microscopy, and chronoamperometry. Compared to commercial Ag nanoparticles, Ag-MOF exhibits superior electrocatalytic CO2RR performance, better stability, and higher catalytic activity. At -0.9 V (vs RHE), the Faraday efficiency of CO achieved 96.1%. When the potential decreased to -1.1 V (vs RHE), the current density could reach 17 mA·cm-2 and the electrode could operate stably for 300 min. It is shown that the chemical environment surrounding the catalytic site can be altered by selecting the appropriate ligand, resulting in the efficient conversion of CO2 to the target product.
Keywords: metal-organic framework  Ag-based metal-organic framework  electrocatalytic CO2 reduction  CO
投稿时间:2023-03-26 修订日期:2023-04-25
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车钰灿,程鹏玮,周毅,柯福生.室温快速合成Ag基金属有机骨架材料用于电催化还原CO2[J].无机化学学报,2023,39(6):1005-1013.
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