Gallium Cluster-Promoted In2O3 Catalyst for CO2 Hydrogenation to Methanol

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-09-06 DOI:10.1021/acscatal.4c03045

Yuxiang Yang, Linlin Wu, Bingqing Yao, Lei Zhang, Munam Jung, Qian He, Ning Yan, Chang-Jun Liu

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引用次数: 0

Abstract

In this work, highly dispersed gallium clusters are constructed on In₂O₃ (denoted as Ga/In₂O₃) to promote hydrogenation of CO₂ to methanol. Compared to pristine In₂O₃, the Ga/In₂O₃ catalysts show markedly improved CO₂ conversion and methanol space-time yield (STY), as well as enhanced stability over 60 h on stream. A strong electronic interaction between the loaded gallium and In₂O₃ support, as confirmed by multiple techniques, results in well-dispersed, stable gallium clusters on In₂O₃, which is beneficial to long-term performance. The interface between gallium clusters and the defective In₂O₃ support serves as active sites to facilitate the activation of H₂ and CO₂. This interfacial synergy not only enhances the adsorption and dissociation of H₂ but also effectively inhibits the strong adsorption of CO₂ as carbonate. The activated CO₂ at the interface sites can be dissociated readily into adsorbed CO for further hydrogenation into methanol.

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镓簇促进的 In2O3 催化剂用于二氧化碳加氢制甲醇

在这项研究中，在 In2O3 上构建了高度分散的镓簇（称为 Ga/In2O3），以促进二氧化碳加氢转化为甲醇。与原始 In2O3 相比，Ga/In2O3 催化剂明显提高了 CO2 转化率和甲醇时空产率（STY），并增强了在 60 小时气流中的稳定性。多种技术证实，负载的镓和 In2O3 载体之间存在强烈的电子相互作用，从而在 In2O3 上形成了分散良好、稳定的镓簇，这有利于催化剂的长期性能。镓团簇与有缺陷的 In2O3 支持物之间的界面是促进 H2 和 CO2 活化的活性位点。这种界面协同作用不仅能增强 H2 的吸附和解离，还能有效抑制 CO2 以碳酸盐形式的强吸附。界面位点上的活化 CO2 很容易解离成吸附的 CO，从而进一步氢化成甲醇。

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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.