调控CuO表面性质选择性电催化还原CO2制HCOOH

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电催化二氧化碳还原反应可将温室气体二氧化碳转化为化工原料或者有机燃料,为克服全球变暖和电能向化学能转化提供了一条可行途径.该技术的主要挑战是产物分布广,导致单一产物选择性低,而调控催化剂的表面性质是解决这一难题的可行策略.本研究通过对氧化亚铜、硫化亚铜进行氧化制备表面性质不同的氧化铜,其中,氧化硫化亚铜制得的CuO-FS催化剂提高了电还原二氧化碳的活性和还原产物甲酸的选择性.该催化剂表现出较高的总电流密度,而且在一个较大的测试电压范围(–0.8~ –1.1 V)内,甲酸的法拉第效率可以保持在70%以上,在–0.9 V时达到最大值78.4%.反应机理探究表明,CuO-FS优异的电还原二氧化碳性能归因于其较大的电化学活性表面积提供了大量表面活性位点,产生较高的总电流密度;而且电催化过程中催化剂表面产生较少的零价Cu,减少了乙烯的生成,使产物更集中于甲酸.
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全球工业化水平的持续提升加速了煤、石油、天然气等化石燃料的消耗, 大量二氧化碳(CO2)被排放进大气, 导致全球变暖和生态失衡, 削减 CO2 排放、将CO2资源化成为亟需解决的问题.2010年前后, 美国、欧洲、日本相继开启以“人工光合成”为题的国家级科研项目, 投入经费均在1亿美元以上.2011年起, 我国国家自然科学基金委、科技部相继资助了相关项目.2020年9月, 我国政府进一步提出力争在2030年前实现“碳达峰”、2060年前实现“碳中和”的目标.
期刊
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21世纪以来,能源短缺和环境污染一直是人类面临的重大挑战?光催化二氧化碳(CO2)还原,通过半导体捕获光能,获得碳氢化合物太阳能燃料是解决能源危机并推动碳循环的有前景的策略之一?然而,活性低?产物选择性差又极大地限制了这一技术的实际应用?因此,调控产物选择性并提高光催化效率、加深对CO2还原反应机理的理解具有重要意义?近年来,超薄材料以其较高的比表面积,丰富的不饱和配位的表面原子,较短的电荷从内部到表面的迁移路径,以及可裁剪的能带结构受到了广泛关注,并在光催化CO2还原领域取得了可喜的成果?本文在总结光催