选择性
催化作用
电催化剂
高分辨率透射电子显微镜
材料科学
可逆氢电极
X射线光电子能谱
化学工程
无机化学
化学
乙烯
电化学
电极
纳米技术
物理化学
透射电子显微镜
工作电极
有机化学
工程类
作者
Gastón O. Larrazábal,Antonio J. Martín,Frank Krumeich,Roland Hauert,Javier Pérez-Ramírez
出处
期刊:Chemsuschem
[Wiley]
日期:2017-02-16
卷期号:10 (6): 1255-1265
被引量:41
标识
DOI:10.1002/cssc.201601578
摘要
The electroreduction of CO2 to fuels and chemicals is an attractive strategy for the valorization of CO2 emissions. In this study, a Cu2 O electrocatalyst prepared by a simple and potentially scalable solvothermal route effectively targeted CO evolution at low-to-moderate overpotentials [with a current efficiency for CO (CECO ) of ca. 60 % after 12 h at -0.6 V vs. reversible hydrogen electrode, RHE], and its selectivity was tuned by the introduction of p-block elements (In, Sn, Ga, Al) into the catalyst. SEM, HRTEM, and voltammetric analyses revealed that the Cu2 O catalyst undergoes extensive surface restructuring (favorable for CO evolution) under the reaction conditions. The modification of Cu2 O with Sn and In further enhanced the current efficiency (CE) for CO (ca. 75 % after 12 h at -0.6 V). In contrast, the introduction of Al altered the selectivity profile of the catalyst significantly, decreasing the selectivity toward CO but promoting the reduction of CO2 to ethylene (CE≈7 %), n-propanol, and ethanol (CE≈2 % each) at -0.8 V vs. RHE. This result is related to a decreased reducibility of Al-doped Cu2 O that might preserve Cu+ species (favorable for C2 H4 production) under the reaction conditions, which is supported by XRD, X-ray photoelectron spectroscopy, and H2 temperature-programmed reduction observations.
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