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在超薄碱式碳酸铋纳米片上修饰石墨炔以促进CO电还原生成甲酸盐。

Decorating graphdiyne on ultrathin bismuth subcarbonate nanosheets to promote CO electroreduction to formate.

作者信息

Tang Shang-Feng, Lu Xiu-Li, Zhang Chao, Wei Zhen-Wei, Si Rui, Lu Tong-Bu

机构信息

MOE International Joint Laboratory of Materials Microstructure, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China.

MOE International Joint Laboratory of Materials Microstructure, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China.

出版信息

Sci Bull (Beijing). 2021 Aug 15;66(15):1533-1541. doi: 10.1016/j.scib.2021.03.020. Epub 2021 Mar 23.

Abstract

Electrocatalytic reduction of CO is one of the most attractive approaches for converting CO into valuable chemical feedstocks and fuels. This work reports a catalyst comprising graphdiyne-decorated bismuth subcarbonate (denoted as BOC@GDY) for efficient electroreduction of CO to formate. The BOC@GDY shows a stable current density of 200 mA cm at -1.1 V in a flow cell configuration, with a faradaic efficiency of 93.5% for formate. Experimental results show that the synergistic effect in BOC@GDY is beneficial for the CO adsorption affinity, the reaction kinetics and the selectivity for formate. In addition, in-situ X-ray absorption and Raman spectroscopy indicate that the electron-rich GDY could facilitate the reduction from Bi(III) to Bi(0), thus leading to more active sites. We also demonstrate that the promoting effect of GDY in CO electroreduction can be further extended to other metal catalysts. To the best of our knowledge, such general promoting functions of GDY for CO electroreduction have not been documented thus far.

摘要

电催化还原CO是将CO转化为有价值的化学原料和燃料最具吸引力的方法之一。这项工作报道了一种由石墨炔修饰的碱式碳酸铋组成的催化剂(表示为BOC@GDY),用于将CO高效电还原为甲酸盐。在流动池配置中,BOC@GDY在-1.1 V时显示出200 mA cm的稳定电流密度,甲酸盐的法拉第效率为93.5%。实验结果表明,BOC@GDY中的协同效应有利于CO的吸附亲和力、反应动力学和对甲酸盐的选择性。此外,原位X射线吸收和拉曼光谱表明,富电子的石墨炔可以促进Bi(III)还原为Bi(0),从而产生更多的活性位点。我们还证明了石墨炔在CO电还原中的促进作用可以进一步扩展到其他金属催化剂。据我们所知,迄今为止尚未记录石墨炔对CO电还原的这种普遍促进作用。

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