室温快速合成Ag基金属有机骨架材料用于电催化还原CO_(2)  

Rapid synthesis of Ag-based metal-organic framework at room temperature for efficient electrocatalytic CO_(2)reduction

作　　者：车钰灿 程鹏玮 周毅 柯福生 CHE Yu‑Can;CHENG Peng‑Wei;ZHOU Yi;KE Fu‑Sheng(College of Chemistry and Molecular Sciences,Wuhan University,Wuhan 430072,China)

机构地区：[1]武汉大学化学与分子科学学院,武汉430072

出　　处：《无机化学学报》2023年第6期1005-1013,共9页Chinese Journal of Inorganic Chemistry

基　　金：国家自然科学基金(No.22172116,21773176)资助。

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CO_(2)反应(CO_(2)RR)。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CO_(2)RR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CO_(2)RR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CO_(2)转化为目标产物。An Ag-based metal-organic framework(Ag-MOF)material was successfully synthesized and used for the first time in the electrocatalytic CO_(2)reduction reaction(CO_(2)RR)by selecting 1,2,4-triazole as the ligand with strong electron-donating ability.The crystal structure,morphology,and electrocatalytic CO_(2)RR 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 CO_(2)RR 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 CO_(2)to the target product.

关 键 词：金属有机骨架 银基金属有机骨架 电催化还原CO_(2) CO 

分 类 号：O614.122[理学—无机化学]