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Construction of High-Density Binuclear Site Catalysts from Double Framework Interfaces at the Cooling Stage
Authors:Shuai Yang  Yao Wei  Xuewen Li  Jianing Mao  Bingbao Mei  Prof. Qing Xu  Prof. Xiaopeng Li  Prof. Zheng Jiang
Affiliation:1. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029 P.R. China

School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201210 P.R. China

These authors contributed equally to this work.;2. Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201800 P.R. China

University of Chinese Academy of Sciences, Beijing, 100049 P.R. China

These authors contributed equally to this work.;3. Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201800 P.R. China

University of Chinese Academy of Sciences, Beijing, 100049 P.R. China;4. Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Science, Shanghai, 201210 P.R. China;5. CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Science, Shanghai, 201210 P.R. China;6. State Key Laboratory for Modification of Chemical Fibers and Polymer Materials & College of Materials Science and Engineering, Donghua University, Shanghai, 201620 P.R. China;7. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029 P.R. China

Abstract:Low-nuclear site catalysts with dual atoms have the potential for applications in energy and catalysis chemistry. Understanding the formation mechanism of dual metal sites is crucial for optimizing local structures and designing desired binuclear sites catalysts. In this study, we demonstrate for the first time the formation process of dual atoms through the pyrolysis of the interface of a double framework using Zn atoms in metal–organic frameworks and Co atoms in covalent organic frameworks. We unambiguously revealed that the cooling stage is the key point to form the binuclear sites by employing the in situ synchrotron radiation X-ray absorption spectrum technique. The binuclear site catalysts show higher activity and selectivity than single dispersed atom catalysts for electrocatalytic oxygen reduction. This work guides us to synthesize and optimize the various binuclear sites for extensive catalytic applications.
Keywords:Binuclear Sites  Oxygen Reduction Reaction  Single Atom Catalysis  X-Ray Absorption Spectrum
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