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
异质结
无机化学
电极
物理化学
参比电极
化学
工程类
生物化学
光电子学
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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