Non‐Precious Metal Catalysts with Gradient Oxidative Dual Sites Boost Bimolecular Activation for Catalytic Oxidation Reactions

Abstract Catalytic oxidation emerges as a highly promising and cost‐effective approach for eliminating gaseous pollutants, greenhouse gases, and volatile organic compounds (VOCs) from industrial exhaust streams. However, achieving the simultaneous activation of O 2 and substrate molecules at low temperatures using non‐precious metal catalysts remains a significant challenge. In this study, we introduce gradient oxidative Cu─O─Ti/Cu─O─Cu dual sites that enhance bimolecular activation for catalytic oxidation reactions. The catalyst, Ti‐doped CuO, is synthesized on a TiO 2 support through the immobilization of Cu 2⁺ on NO 3 ⁻‐grafted TiO 2 , followed by thermal treatment. The resulting gradient oxidative Cu─O─Ti/Cu─O─Cu sites exhibit exceptional catalytic oxidation activity for NH 3 and various VOCs at low temperatures, matching the performance of precious metal‐based catalysts. Notably, during NH₃ oxidation, Cu─O─Ti sites enhance the activation of both O₂ and NH₃. HNO intermediates formed on Cu─O─Ti sites react with NH intermediates on neighboring Cu─O─Cu sites—producing N₂ and H₂O via an imide mechanism—which effectively lowers the reaction barrier for catalytic NH₃ oxidation. As such, dual sites in non‐precious metal catalysts show promising results for advancing future catalytic oxidation technologies.

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Publication Details

Journal
Angewandte Chemie
Published
2025-04-09
DOI
https://doi.org/10.1002/ange.202506018
Primary Topic
Metal-Organic Frameworks: Synthesis and Applications
Type
article
Field-Weighted Citation Impact
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article

Non‐Precious Metal Catalysts with Gradient Oxidative Dual Sites Boost Bimolecular Activation for Catalytic Oxidation Reactions

Xiaoya Xue, Ming Xie, Xingchi Li, Mengxue Wang et al.
Angewandte Chemie
Metal-Organic Frameworks: Synthesis and Applications
article

Non‐Precious Metal Catalysts with Gradient Oxidative Dual Sites Boost Bimolecular Activation for Catalytic Oxidation Reactions

Xiaoya Xue, Ming Xie, Xingchi Li, Mengxue Wang, Dengsong Zhang, Evangelina Pensa, Yongjie Shen, Emiliano Cortés, Tianwei Lan, Yanqing Li, Lupeng Han, Zixiang Xu, Xin Chen, Yufei Wang
article en

Abstract

Abstract Catalytic oxidation emerges as a highly promising and cost‐effective approach for eliminating gaseous pollutants, greenhouse gases, and volatile organic compounds (VOCs) from industrial exhaust streams. However, achieving the simultaneous activation of O 2 and substrate molecules at low temperatures using non‐precious metal catalysts remains a significant challenge. In this study, we introduce gradient oxidative Cu─O─Ti/Cu─O─Cu dual sites that enhance bimolecular activation for catalytic oxidation reactions. The catalyst, Ti‐doped CuO, is synthesized on a TiO 2 support through the immobilization of Cu 2⁺ on NO 3 ⁻‐grafted TiO 2 , followed by thermal treatment. The resulting gradient oxidative Cu─O─Ti/Cu─O─Cu sites exhibit exceptional catalytic oxidation activity for NH 3 and various VOCs at low temperatures, matching the performance of precious metal‐based catalysts. Notably, during NH₃ oxidation, Cu─O─Ti sites enhance the activation of both O₂ and NH₃. HNO intermediates formed on Cu─O─Ti sites react with NH intermediates on neighboring Cu─O─Cu sites—producing N₂ and H₂O via an imide mechanism—which effectively lowers the reaction barrier for catalytic NH₃ oxidation. As such, dual sites in non‐precious metal catalysts show promising results for advancing future catalytic oxidation technologies.

Angewandte ChemieVol. 137(25)
Shanghai University (CN), Hokkaido University (JP), Shanghai Advanced Research Institute (CN), University of Bath (GB), Ludwig-Maximilians-Universität München (DE)
Openalex Percentile: Top 94%
Metal-Organic Frameworks: Synthesis and Applications
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