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利用锚定的铋单原子提高甲酸根对一氧化碳还原的选择性。

Boost Selectivity of HCOO Using Anchored Bi Single Atoms towards CO Reduction.

作者信息

Yang Xupeng, Chen Yuliang, Qin Lang, Wu Xiaonan, Wu Yuting, Yan Tao, Geng Zhigang, Zeng Jie

机构信息

Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.

出版信息

ChemSusChem. 2020 Dec 7;13(23):6307-6311. doi: 10.1002/cssc.202001609. Epub 2020 Sep 3.

DOI:10.1002/cssc.202001609
PMID:32755063
Abstract

Single atoms have been widely applied as efficient catalysts in various catalytic systems due to its high selectivity for certain products, which is induced by a uniform coordinate environment of active sites. Herein, it is demonstrated that Bi single atoms anchored on carbon black (Bi SAs/C) can serve as an efficient catalyst for CO electroreduction into formate (HCOO ). During CO electroreduction, Bi SAs/C achieved a faradaic efficiency for HCOO of 83.6 % at-1.1 Vversus reversible hydrogen electrode (V vs. RHE). Notably, the selectivity for HCOO of Bi SAs/C was always higher than 95 % at all applied potentials. In addition, at-1.2 Vvs.RHE, the current density for HCOO formation in thepresence of Bi SAs/C reached-12.0 mA cm , which was 3.4 times as high as that (-3.5 mA cm ) of BiO clusters on carbon black (BiO /C). Mechanistic studies revealed that Bi SAs/C facilitated the faradaic process and accelerated reaction kinetics in comparison with BiO /C.

摘要

由于活性位点的均匀配位环境导致对某些产物具有高选择性,单原子已在各种催化体系中被广泛用作高效催化剂。在此,证明了锚定在炭黑上的铋单原子(Bi SAs/C)可作为将CO电还原为甲酸盐(HCOO⁻)的高效催化剂。在CO电还原过程中,Bi SAs/C在相对于可逆氢电极(V vs. RHE)为-1.1 V时实现了HCOO⁻的法拉第效率为83.6%。值得注意的是,在所有施加电位下,Bi SAs/C对HCOO⁻的选择性始终高于95%。此外,在-1.2 V vs. RHE时,存在Bi SAs/C时HCOO⁻形成的电流密度达到-12.0 mA cm⁻²,是炭黑上BiO簇(BiOₓ/C)的电流密度(-3.5 mA cm⁻²)的3.4倍。机理研究表明,与BiOₓ/C相比,Bi SAs/C促进了法拉第过程并加速了反应动力学。

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