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Dynamic restructuring induced Cu nanoparticles with ideal nanostructure for selective multi-carbon compounds production via carbon dioxide electroreduction
Journal of Catalysis ( IF 6.5 ) Pub Date : 2020-01-24 , DOI: 10.1016/j.jcat.2020.01.002
Zhe Xu , Tiancheng Wu , Yu Cao , Congcong Chen , Xierong Zeng , Peng Lin , Wei-Wei Zhao

Production of multi-carbon (C2+) products via electrochemical CO2 reduction reaction (CO2RR) has aroused intensive interest in this decade. However, it is still a great challenge in large-scale synthesis of electrocatalysts for C2+ compounds production with high selectivity and rate in neutral electrolyte. In this study, a robust and scalable aqueous synthesis method was proposed to prepare CuO nanosheets, which was directly used as CO2RR electrocatalyst. The catalyst underwent dynamic restructuring during the pre-reduction stage, which significantly changed the morphology, crystalline structure and electrochemical properties of the catalyst. As a result, the pristine CuO nanosheets gradually evolved to coral-like Cu nanoparticle ensembles (CL-Cu NEs). In 0.1 M KHCO3 at −1.1 V vs. RHE, the CL-Cu NEs exhibited a faradaic efficiency and partial current density of C2+ products of 72.1% and 25.2 mA cm−2 respectively and no degradation was observed in 15 h running. In contrast to many Cu-based catalysts showing considerable C2+ products selectivity, the (sub)surface oxygen and Cu+ species were unlikely to play a significant role in this study. The strong performance of CL-Cu NEs was ascribed to the synergism between the coral-like morphology and abundant Cu(1 0 0)/Cu(1 1 1) interfaces. This methodology may provide a cost-effective approach for large-scale preparation of CO2RR electrocatalysts with ideal nanostructure.



中文翻译:

动态重组诱导的具有理想纳米结构的Cu纳米颗粒,用于通过二氧化碳电还原选择性生产多种碳化合物

通过电化学CO 2还原反应(CO 2 RR)生产多碳(C 2+)产品引起了这一十年的浓厚兴趣。然而,在大规模合成用于中性电解质中具有高选择性和速率的C 2+化合物生产的电催化剂方面,仍然是一个巨大的挑战。在这项研究中,提出了一种鲁棒且可扩展的水合成方法来制备直接用作CO 2的CuO纳米片。RR电催化剂。催化剂在预还原阶段进行了动态重组,从而显着改变了催化剂的形态,晶体结构和电化学性能。结果,原始的CuO纳米片逐渐演化为珊瑚状的Cu纳米粒子集合体(CL-Cu NEs)。在相对于RHE为-1.1 V的0.1 M KHCO 3中,CL-Cu NEs的法拉第效率和C 2+产物的部分电流密度分别为72.1%和25.2 mA cm -2,并且在15 h运行中未观察到降解。与许多显示出相当高的C 2+产物选择性的铜基催化剂相比,(亚)表面氧和Cu +物种不太可能在这项研究中发挥重要作用。CL-Cu NEs的强大性能归因于珊瑚状形态与丰富的Cu(1 0 0)/ Cu(1 1 1)界面之间的协同作用。该方法可以为大规模制备具有理想纳米结构的CO 2 RR电催化剂提供一种经济有效的方法。

更新日期:2020-01-26
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