材料科学
电化学
催化作用
电催化剂
法拉第效率
氧化还原
化学工程
X射线光电子能谱
可逆氢电极
电解质
无机化学
电极
物理化学
参比电极
生物化学
工程类
化学
冶金
作者
Dong Xiang,Kunzhen Li,Manzhi Li,Ran Long,Yujie Xiong,Dmitry G. Yakhvarov,Xiongwu Kang
标识
DOI:10.1016/j.mtphys.2023.101045
摘要
Rational design of high performance electrocatalyst towards electrochemical CO2 reduction (CO2RR) to C2 products remains a grand challenge. Herein, a heterostructured [email protected]0.4W0.6 catalyst was designed under the guidance of theoretical calculation towards CO2RR to C2 products and prepared by sequential reverse microemulsion and thermal reduction. The heterostructure of [email protected]0.4W0.6 catalysts were corroborated by X-ray diffraction (XRD) and transmission electron microscopy (TEM), which displayed spherical shape and a size of 15.6 ± 0.5 nm. X-ray photoelectron spectroscopy illustrated more electron transfer from copper (Cu) to tungsten (W) in heterostructured [email protected]0.4W0.6 catalyst than that pure Cu0.4W0.6. The pure Cu0.4W0.6 catalyst is dominated by hydrogen evolution in CO2RR, while heterostructured [email protected]0.4W0.6 catalyst show much enhanced selectivity and activity towards C2 products, which is strongly dependent on the mass ratio of Cu to Cu0.4W0.6, ascribing to the Cu/Cu0.4W0.6 interface. Eventually, the [email protected]0.4W0.6 champion catalyst displays a Faradaic efficiency (FE) of 60.9% and a partial current density of 121.8 mA cm−2 at −1.0 V (vs. RHE) for C2 products in CO2RR in alkaline electrolyte. Computational studies indicated that the heterostructured [email protected]0.4W0.6 suppresses hydrogen evolution and favors the production of CO and asymmetrical CO–CHO coupling, ascribing to the charge redistribution at the Cu/Cu0.4W0.6 interface. The high O affinity of W facilitates the rupture of C–O bond of *C2H3O intermediate and promotes the formation of ethylene. In-situ Raman spectroscopy revealed high surface coverage of bridging *CO and *CO–CHO intermediate for C2 products at 2660 cm−1 on [email protected]0.4W0.6, corroborating the CO–CHO coupling mechanism. This work highlights the importance of heterostructured Cu-based catalysts in tuning the CO2RR activity and selectivity of Cu-based materials.
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