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나노물질및화학반응연구단
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Tuning CO2 Hydrogenation Selectivity through Reaction-Driven Restructuring on Cu-Ni Bimetal Catalysts

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Title
Tuning CO2 Hydrogenation Selectivity through Reaction-Driven Restructuring on Cu-Ni Bimetal Catalysts
Author(s)
Kasala Prabhakar Reddy; Daeho Kim; Seunghwa Hong; Kim, Ki-Jeong; Ryoo, Ryong; Jeong Young Park
Publication Date
2023-02
Journal
ACS Applied Materials & Interfaces, v.15, no.7, pp.9373 - 9381
Publisher
American Chemical Society
Abstract
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 gamma-Al2O3 was performed to increase CO selectivity while maintaining the high reaction rate. The Cu0.5Ni0.5/gamma-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.
URI
https://pr.ibs.re.kr/handle/8788114/13099
DOI
10.1021/acsami.2c20832
ISSN
1944-8244
Appears in Collections:
Center for Nanomaterials and Chemical Reactions(나노물질 및 화학반응 연구단) > 1. Journal Papers (저널논문)
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