Zhang Bin-Bin, Wang Ya-Hui, Xu Shan-Min, Chen Kai, Yang Yu-Guo, Kong Qing-Hua
Department of Chemistry, School of Science, Beijing Jiaotong University Beijing 100044 China
RSC Adv. 2020 May 20;10(33):19192-19198. doi: 10.1039/d0ra02482a.
The electrosynthesis of high-value ethanol from carbon dioxide and carbon monoxide addresses the need for the large-scale storage of renewable electricity and reduction of carbon emissions. However, the electrosynthesis of ethanol by the CO reduction reaction (CORR) has suffered from low selectivity and energy efficiency. Here, we report a catalyst composed of Au nanoparticles in CuO nanocavities (Au@CuO) that is very active for CO reduction to ethanol through the confinement of the CO intermediate. The architecture shows tandem catalysis mechanisms in which CO reduction on Au yolks produces CO filling Cu nanocavities, where a sufficiently high CO concentration due to the confinement effect promotes ethanol formation and then results in an ethanol faradaic efficiency of 52.3% at -0.30 V the reversible hydrogen electrode ( RHE) regulating the hollow size of the CuO nanocavities. Such a strategy provides a new way of fabricating various tandem catalysts with high selectivity and efficiency for the CORR.
通过二氧化碳和一氧化碳电合成高价值乙醇满足了大规模存储可再生电力和减少碳排放的需求。然而，通过CO还原反应（CORR）电合成乙醇存在选择性低和能量效率低的问题。在此，我们报道了一种由CuO纳米腔中的Au纳米颗粒组成的催化剂（Au@CuO），该催化剂通过限制CO中间体对将CO还原为乙醇具有很高的活性。该结构显示出串联催化机制，其中Au核上的CO还原产生填充Cu纳米腔的CO，由于限制效应导致足够高的CO浓度促进乙醇形成，进而在-0.30 V（相对于可逆氢电极（RHE））时乙醇法拉第效率达到52.3%，通过调节CuO纳米腔的中空尺寸实现。这种策略为制备用于CORR的具有高选择性和效率的各种串联催化剂提供了一种新方法。
