Mo-Bi双金属硫化物纳米层片用于高效电化学催化CO_2制备甲醇的研究
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摘要
CO_2回收及利用具有能源、环境、经济多重意义,同时也是控制全球气候变暖的一项紧迫任务。电化学催化还原的方法可以在温和条件下使CO_2还原为一氧化碳、烃类、酸类、醇类等高附加值的精细化工产品。而电极材料是决定还原产物和效率的重要因素。本工作通过溶剂热的方法制备了Mo-Bi双金属硫化物纳米层片,采用SEM、TEM、XPS和DLS等手段对其结构性能进行了系统的研究。以碳纸为基底、Mo-Bi双金属硫化物纳米层片作为阴极电催化材料、1-丁基-3-甲基咪唑四氟硼酸盐的乙腈溶液作为电解质,可以高效催化转化CO_2为甲醇。结果表明,这一体系中甲醇的法拉第效率最高可以达到71.2%,同时甲醇的还原电流密度可达到12.1 mA cm~(-2)。其可能的反应路径为CO_2→CO_2~-→CO_(ad)→CHO_(ads)→CH_3O_(ads)→甲醇。
CO_2 is cheap,abundant and safe carbon resource,and its transformation into valuable chemicals and fuel has received much attention.Methanol is a very useful chemical.We carried out the first work to use Mo-Bi bimetallic chalcogenide as electrocatalyst for CO_2 reduction.By using the Mo-Bi BMC on carbon paper as electrode and l-butyl-3-methylimidazolium tetrafluoroborate in acetonitrile as electrolyte,the Faradaic efficiency of methanol could reach 71.2%with a current density of 12.1 mA cm~(-2),which is much higher than the best result reported to date.Detailed study indicates that the outstanding performance of the electrode resulted from the excellent synergistic effect of Mo and Bi for producing methanol.
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