In Situ Dynamic Structural Changes of Ruthenium-Loaded MoO3 for Photothermal Catalytic CO2 Reduction

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-06-16 DOI:10.1021/acscatal.5c02307

Dongdong Chu, Mingkai Xu, Yunjie Zou, Chao Xing, Dayu Sun, Lan Ling

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Abstract

Hydrogen spillover has been widely recognized as a pivotal phenomenon in heterogeneous catalysis, yet the global impact of active hydrogen species on support materials remains underexplored, hindering the establishment of robust structure–performance correlations. In this study, we employed in situ scanning transmission electron microscopy (in situ STEM) to investigate the support effect in ruthenium-loaded molybdenum trioxide (Ru/MoO₃) catalysts during the reversed water–gas shift reaction (RWGS). Our observations revealed that the presence of active hydrogen atoms markedly enhanced the evolution of lattice oxygen from MoO₃, resulting in the transformation of the Ru-MoO₃ nanosheet into a porous structure reminiscent of a jigsaw puzzle, thereby creating active CO₂ sites on the catalytic surface. The controlled surface reconstruction of Ru-MoO₃ enabled 14.3% CO₂ conversion and nearly 100% CO selectivity at 300 °C, closely approaching the thermodynamic equilibrium limit of the RWGS reaction. These findings provide critical insights into the influence of active hydrogen on the morphology and crystal structure of supports at a comprehensive scale, underscoring its potential to enhance photothermal catalytic CO₂ hydrogenation performance and paving the way for the development of more efficient CO₂ conversion technologies.

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载钌MoO3光热催化CO2还原的原位动态结构变化

氢溢出已被广泛认为是多相催化中的关键现象，但活性氢对支撑材料的全球影响仍未得到充分研究，这阻碍了结构-性能相关性的建立。在本研究中，我们采用原位扫描透射电子显微镜（In situ STEM）研究了负载钌的三氧化钼（Ru/MoO3）催化剂在逆向水气转换反应（RWGS）中的支撑效应。我们的观察表明，活性氢原子的存在显著增强了MoO3晶格氧的演化，导致Ru-MoO3纳米片转变为类似拼图游戏的多孔结构，从而在催化表面产生活性CO2位点。在300℃下，Ru-MoO3的可控表面重构使CO2转化率达到14.3%，CO选择性接近100%，接近RWGS反应的热力学平衡极限。这些发现为全面了解活性氢对载体形态和晶体结构的影响提供了重要见解，强调了其增强光热催化CO2加氢性能的潜力，并为开发更高效的CO2转化技术铺平了道路。

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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.