Room-Temperature CO Oxidative Coupling for Oxamide Production over Interfacial Au/ZnO CatalystsClick to copy article linkArticle link copied!
- Yanwei CaoYanwei CaoState Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics (LICP), Chinese Academy of Sciences, Lanzhou 730000, ChinaCollaborative Innovation Center of Chemistry for Energy Material, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Key Laboratory of Computational Physical Science, Department of Chemistry, Fudan University, Shanghai 200433, ChinaMore by Yanwei Cao
- Yao PengYao PengCollaborative Innovation Center of Chemistry for Energy Material, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Key Laboratory of Computational Physical Science, Department of Chemistry, Fudan University, Shanghai 200433, ChinaMore by Yao Peng
- Danyang ChengDanyang ChengCollege of Chemistry and Molecular Engineering and College of Engineering, Peking University, Beijing 100871, ChinaMore by Danyang Cheng
- Lin ChenLin ChenCollaborative Innovation Center of Chemistry for Energy Material, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Key Laboratory of Computational Physical Science, Department of Chemistry, Fudan University, Shanghai 200433, ChinaMore by Lin Chen
- Maolin WangMaolin WangCollege of Chemistry and Molecular Engineering and College of Engineering, Peking University, Beijing 100871, ChinaMore by Maolin Wang
- Cheng ShangCheng ShangCollaborative Innovation Center of Chemistry for Energy Material, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Key Laboratory of Computational Physical Science, Department of Chemistry, Fudan University, Shanghai 200433, ChinaMore by Cheng Shang
- Lirong ZhengLirong ZhengBeijing Synchrotron Radiation Facility (BSRF), Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, ChinaMore by Lirong Zheng
- Ding Ma*Ding Ma*Email: [email protected]College of Chemistry and Molecular Engineering and College of Engineering, Peking University, Beijing 100871, ChinaMore by Ding Ma
- Zhi-Pan Liu*Zhi-Pan Liu*Email: [email protected]Collaborative Innovation Center of Chemistry for Energy Material, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Key Laboratory of Computational Physical Science, Department of Chemistry, Fudan University, Shanghai 200433, ChinaMore by Zhi-Pan Liu
- Lin He*Lin He*Email: [email protected]State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics (LICP), Chinese Academy of Sciences, Lanzhou 730000, ChinaMore by Lin He
Abstract
The conversion of carbon monoxide (CO) into high-value organic molecules has long been pursued by both industry and academia. One of the central challenges is to realize carbon–carbon coupling with high selectivity for CO insertion. We report here a highly selective Au/ZnO composite catalyst for one-step oxidative coupling of CO with secondary amines, producing oxamides. The reaction is >99% selective under ambient conditions, which exhibits a subtle change of catalyst activity over ∼120 h in a fixed-bed reactor. A combination of microscopic and spectroscopic studies (including X-ray photoemission spectroscopy, X-ray absorption spectroscopy, CO-Fourier transform infrared spectroscopy, and aberration-corrected high-angle annular dark-field scanning transmission electron microscopy) and machine learning reveal that the active site is the Au–ZnO interface with a Au nanocluster attached to the ZnO support via nonstoichiometric ZnOx (x > 1) linkages. The reaction mechanism and key reaction intermediates were confirmed by density functional theory calculations and in situ diffused reflectance infrared Fourier transform spectroscopy signals. Our results open an avenue in heterogeneous catalysis to achieve the ambient-condition CO transformation by exploiting the interfacial synergistic effects.
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