Uncovering the synergy between gold and sodium on ZrO2 for boosting the reverse water gas shift reaction: In-situ spectroscopic investigations

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2024-01-03 DOI:10.1016/j.apcatb.2023.123685

Abdallah I.M. Rabee , Sebastian Cisneros , Dan Zhao , Carsten R. Kreyenschulte , Stephan Bartling , Vita Kondratenko , Christoph Kubis , Evgenii V. Kondratenko , Angelika Brückner , Jabor Rabeah

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Abstract

CO₂ conversion to CO via the reverse water-gas shift (RWGS) reaction is a promising source of syngas for subsequent synthesis of liquid fuels and chemicals. Herein, we present the synthesis of catalysts containing Au supported on hydroxylated Na-modified ZrO₂, with Au amounts ranging from 0.05 to 1 wt%. Systematic investigations reveal the formation of cooperative Au/Na sites at the interface. These sites cooperate synergistically to activate CO₂ and generate a high surface density of carboxylate-like species, which serve as highly active intermediates for CO formation. It was found that the RWGS reaction on the catalyst with low Au loading proceeds mainly via a carboxylate pathway, with bidentate formate acting as spectators. At higher Au loading, the bidentate formate pathway contributes somewhat to CO formation alongside the carboxylate pathway. Based on temporal analysis of products, we emphasize the significant roles of H₂ spillover and the metal-support interface in the RWGS reaction.

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揭示 ZrO2 上金和钠在促进反向水气变换反应中的协同作用：原位光谱研究

通过反向水气变换（RWGS）反应将二氧化碳转化为一氧化碳是一种很有前景的合成气来源，可用于后续液体燃料和化学品的合成。在此，我们介绍了在羟化 Na 改性 ZrO2 上支撑的含金催化剂的合成，金的含量从 0.05 到 1 wt.%。系统研究表明，在界面上形成了金/纳协同位点。这些位点协同激活了二氧化碳，并产生了高密度的羧酸盐类物质，成为二氧化碳形成的高活性中间体。研究发现，在金负载量较低的催化剂上，RWGS 反应主要通过羧酸盐途径进行，而双叉甲酸盐则充当旁观者。金负载量较高时，双叉甲酸酯途径与羧酸酯途径一起在一定程度上促进了 CO 的形成。根据对产物的时间分析，我们强调了 H2 溢出和金属-支撑界面在 RWGS 反应中的重要作用。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.