Formation of Copper Catalysts for CO2 Reduction with High Ethylene/Methane Product Ratio Investigated with In Situ X-ray Absorption Spectroscopy
Formation of Copper Catalysts for CO2 Reduction with High Ethylene/Methane Product Ratio Investigated with In Situ X-ray Absorption Spectroscopy
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DOI：
10.1021/acs.jpclett.6b00367
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发表时间：
2016-04-21
影响因子：
5.7
通讯作者：
Nilsson, Anders
中科院分区：
文献类型：
--
作者：
Eilert, Andre;Roberts, F. Sloan;Nilsson, Anders
纳米结构铜阴极是迄今为止最有效和最有选择性的催化剂之一，用于从电化学二氧化碳还原反应(CO2RR)中制备多碳产品。我们报道了一种高活性的铜纳米立方体CO_2RR催化剂的形成的原位X射线吸收光谱研究，该催化剂比甲烷的生成更有利于乙烯的产生。结果表明，铜纳米立方体形成的前驱体是铜(I)-氧化物，而不是先前假设的铜(I)-氯化物。还报道了通过铜(II)-碳酸盐/氢氧化物获得电化学相似材料的第二种途径。本研究强调了使用氧化铜前驱体构建选择性CO2还原催化剂的重要性，并表明前驱体的氧化状态不影响电催化剂对乙烯生成的选择性。
Nanostructured copper cathodes are among the most efficient and selective catalysts to date for making multicarbon products from the electrochemical carbon dioxide reduction reaction (CO2RR). We report an in situ X-ray absorption spectroscopy investigation of the formation of a copper nanocube CO2RR catalyst with high activity that highly favors ethylene over methane production. The results show that the precursor for the copper nanocube formation is copper(I)-oxide, not copper(I)-chloride as previously assumed. A second route to an electrochemically similar material via a copper(II)-carbonate/hydroxide is also reported. This study highlights the importance of using oxidized copper precursors for constructing selective CO2 reduction catalysts and shows the precursor oxidation state does not affect the electrocatalyst selectivity toward ethylene formation.