双金属片
选择性
催化作用
材料科学
X射线光电子能谱
双金属
镍
纳米颗粒
微型反应器
化学工程
无机化学
金属
纳米技术
化学
冶金
有机化学
工程类
作者
Kasala Prabhakar Reddy,Daeho Kim,Seunghwa Hong,Ki-Jeong Kim,Ryong Ryoo,Jeong Young Park
标识
DOI:10.1021/acsami.2c20832
摘要
Tuning the selectivity of CO2 hydrogenation is of significant scientific interest, especially using nickel-based catalysts. Fundamental insights into CO2 hydrogenation on Ni-based catalysts demonstrate that CO is a primary intermediate, and product selectivity is strongly dependent on the oxidation state of Ni. Therefore, modifying the electronic structure of the nickel surface is a compelling strategy for tuning product selectivity. Herein, we synthesized well dispersed Cu–Ni bimetallic nanoparticles (NPs) using a simple hydrothermal method for CO selective CO2 hydrogenation. A detailed study on the monometallic (Ni and Cu) and bimetallic (CuxNi1–x) catalysts supported on γ-Al2O3 was performed to increase CO selectivity while maintaining the high reaction rate. The Cu0.5Ni0.5/γ-Al2O3 catalyst shows a high CO2 conversion and more CO product selectivity than its monometallic counterparts. The surface electronic and geometric structure of Cu0.5Ni0.5 bimetallic NPs was studied using ambient pressure X-ray photoelectron spectroscopy (AP-XPS) and in situ diffuse reflectance infrared Fourier-transform spectroscopy under reaction conditions. The Cu core atoms migrate toward the surface, resulting in the restructuring of the Cu@Ni core–shell structure to a Cu–Ni alloy during the reaction and functioning as the active site by enhancing CO desorption. A systematic correlation is obtained between catalytic activity from a continuous fixed-bed flow reactor and the surface electronic structural details derived from AP-XPS results, establishing the structure–activity relationship. This investigation contributes to providing a strategy for controlling CO2 hydrogenation selectivity by modifying the surface structure of bimetallic NP catalysts.
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