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Stable and selective electrochemical reduction of carbon dioxide to ethylene on copper mesocrystals

机译：在铜中晶体上将二氧化碳二氧化碳降低到乙烯的稳定和选择性的电化学还原

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摘要

Stable and selective electrochemical reduction of carbon dioxide to ethylene was achieved using copper mesocrystal catalysts in 0.1 M KHCO3. The Cu mesocrystal catalysts were facilely derived by the in situ reduction of a thin CuCl film during the first 200 seconds of the CO2 electroreduction process. At -0.99 V vs. RHE, the Faradaic efficiency of ethylene formation using these Cu mesocrystals was similar to 18x larger than that of methane and forms up to 81% of the total carbonaceous products. Control CO2 reduction experiments show that this selectivity towards C2H4 formation could not be replicated by using regular copper nanoparticles formed by pulse electrodeposition. High resolution transmission electron microscopy reveals the presence of both (100)(Cu) facets and atomic steps in the Cu mesocrystals which we assign as active sites in catalyzing the reduction of CO2 to C2H4. CO adsorption measurements suggest that the remarkable C2H4 selectivity could be attributed to the greater propensity of CO adsorption on Cu mesocrystals than on other types of Cu surfaces. The Cu mesocrystals remained active and selective towards C2H4 formation for longer than six hours. This is an important and industrially relevant feature missing from many reported Cu-based CO2 reduction catalysts.
机译：使用0.1 M KHCO3中的铜中晶催化剂实现了二氧化碳为乙烯的稳定和选择性的电化学还原。 CU中晶催化剂是通过在二氧化碳电动过程的前200秒内的原位减少薄膜的原位减少来衍生得出的。在-0.99 V与Rhe的情况下，使用这些Cu中晶的乙烯形成的法拉达效率类似于甲烷的18倍，并形成多达81％的总碳质产物。对照CO2还原实验表明，对C2H4形成的这种选择性无法通过使用脉冲电沉积形成的常规铜纳米颗粒来复制。高分辨率的透射电子显微镜揭示了CU中晶中的（100）（CU）方面和原子步骤的存在，我们将其分配为活跃位点，以催化将CO2降低到C2H4。 CO吸附测量表明，与其他类型的Cu表面相比，CO上吸附的CO吸附倾向更大，可以归因于CO上吸附的倾向更大。 Cu介质晶体保持活跃，对C2H4形成的选择性超过六小时。这是许多报道的基于CU的CO2还原催化剂所缺少的重要且与工业相关的功能。

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