Wang Pengtang, Yang Hao, Tang Cheng, Wu Yu, Zheng Yao, Cheng Tao, Davey Kenneth, Huang Xiaoqing, Qiao Shi-Zhang
School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005, Australia.
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
Nat Commun. 2022 Jun 29;13(1):3754. doi: 10.1038/s41467-022-31427-9.
Electroreduction of carbon dioxide (CO) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically low because of limited selectivity, especially under high current operation. Here we report a new silver-modified copper-oxide catalyst (dCuO/Ag) that exhibits a significant Faradaic efficiency of 40.8% and energy efficiency of 22.3% for boosted EtOH production. Importantly, it achieves CO-to-ethanol conversion under high current operation with partial current density of 326.4 mA cm at -0.87 V vs reversible hydrogen electrode to rank highly significantly amongst reported Cu-based catalysts. Based on in situ spectra studies we show that significantly boosted production results from tailored introduction of Ag to optimize the coordinated number and oxide state of surface Cu sites, in which the CO adsorption is steered as both atop and bridge configuration to trigger asymmetric C-C coupling for stablization of EtOH intermediates.
将二氧化碳（CO₂）电还原为多碳产物为大规模化学品生产提供了可能性，因此具有重大的研究和商业价值。然而，乙醇（EtOH）作为一种重要的化学原料，其生产效率由于选择性有限而低得难以实际应用，尤其是在高电流操作下。在此，我们报道了一种新型的银修饰氧化铜催化剂（dCuO/Ag），该催化剂在促进乙醇生产方面表现出显著的法拉第效率40.8%和能量效率22.3%。重要的是，它在高电流操作下实现了CO₂到乙醇的转化，相对于可逆氢电极，在-0.87 V时的分电流密度为326.4 mA cm⁻²，在已报道的铜基催化剂中排名非常靠前。基于原位光谱研究，我们表明产量的显著提高源于银的定制引入，以优化表面铜位点的配位数和氧化态，其中CO的吸附以顶位和桥式构型进行引导，从而触发不对称C-C偶联以稳定乙醇中间体。
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