Revisiting the Morphology-Dependent CO2 Hydrogenation over Ru/CeO2 Catalysts

IF 13.6 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2026-07-17 Epub Date: 2026-06-30 DOI:10.1021/acscatal.6c03659

Fangxian Cao*, Zhuowen Li, Bingzhang Li, Jianjun Chen, Jiangping Liu*, Sai Zhang* and Xiao-Dong Wen*,

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引用次数: 0

Abstract

The morphologies of CeO₂ nanocrystals significantly influence the Ru-catalyzed CO₂ hydrogenation. However, the morphology-dependent catalytic behaviors remain controversial and poorly understood. In this study, three shape-specific CeO₂-supported Ru catalysts (cubes, polyhedra, and rods) were successfully synthesized, and then, the origin of morphology effects on Ru-catalyzed CO₂ hydrogenation was systematically investigated by means of ex situ/in situ characterizations. The cubic CeO₂-supported Ru catalyst exhibited the highest CO₂ conversion rate and CH₄ selectivity. In situ DRIFTS revealed that CO₂ hydrogenation over Ru/CeO₂ proceeds via the formate and carbonyl routes, with the former being favored at lower temperatures. The detailed characterizations demonstrated that the morphology-dependent metal–support interaction (MSI) influences the chemical states of Ru species, thereby regulating the adsorption/activation of H₂ and the CO* intermediate, which ultimately determines the catalytic activity and selectivity in CO₂ hydrogenation. This study highlighted that the MSI strength, rather than oxygen vacancies, serves as a key descriptor governing the catalytic performance.

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Ru/CeO2催化剂上形态依赖的CO2加氢研究

CeO2纳米晶的形貌对ru催化CO2加氢有显著影响。然而，形态依赖的催化行为仍然存在争议，并且知之甚少。在本研究中，成功合成了三种形状特定的ceo2负载Ru催化剂（立方体、多面体和棒状），并通过非原位/原位表征系统地研究了Ru催化CO2加氢的形貌影响来源。立方体ceo2负载Ru催化剂表现出最高的CO2转化率和CH4选择性。原位漂移表明，Ru/CeO2上的CO2加氢通过甲酸和羰基途径进行，前者在较低温度下更有利。详细表征表明，形态依赖的金属-载体相互作用（MSI）影响Ru的化学状态，从而调节H2和CO*中间体的吸附/活化，最终决定了CO2加氢的催化活性和选择性。这项研究强调了MSI强度，而不是氧空位，是控制催化性能的关键描述符。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.