Cation-Exchange Induced Precise Regulation of Single Copper Site Triggers Room-Temperature Oxidation of Benzene,Journal of the American Chemical Society

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Cation-Exchange Induced Precise Regulation of Single Copper Site Triggers Room-Temperature Oxidation of Benzene
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2020-06-25 , DOI: 10.1021/jacs.0c03415
Huang Zhou ₁ , Yafei Zhao ₁ , Jie Gan ₂ , Jie Xu ₃ , Ying Wang _{4,

5} , Hongwei Lv ₁ , Shi Fang ₆ , Zhiyuan Wang ₁ , Ziliang Deng ₃ , Xiaoqian Wang ₁ , Peigen Liu ₁ , Wenxin Guo ₁ , Boyang Mao ₇ , Huijuan Wang ₈ , Tao Yao ₆ , Xun Hong ₁ , Shiqiang Wei ₆ , Xuezhi Duan ₂ , Jun Luo ₃ , Yuen Wu ₁

Affiliation

Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, and National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230026, China.
State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China.
Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials & Low-Carbon Technologies, Tianjin University of Technology, Tianjin 300384, China.
State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China.
Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, P.R. China.
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230026, China.
National Graphene Institute, University of Manchester, Booth Street East, Manchester M13 9PL, United Kingdom.
Center for Micro and Nanoscale Research and Fabrication, University of Science and Technology of China, Hefei, Anhui 230026, China.

The controllable synthesis of stable single-metal site catalysts with an expected coordination environment for high catalytic activity and selectivity is still challenging. Here, we propose a cation-exchange strategy for precise production of an edge-rich sulfur (S) and nitrogen (N) dual-decorated single-metal (M) site catalysts (M = Cu, Pt, Pd, etc.) library. Our strategy relies on the anionic frameworks of sulfides and N-rich polymer shell to generate abundant S and N defects during high-temperature annealing, further facilitating the stabilization of exchanged metal species with atomic dispersion and excellent accessibility. This process was traced by in-situ transmission electron microscopy, during which no metal aggregates were observed. Both experiments and theoretical results reveal the precisely obtained S, N dual-decorated Cu sites exhibit a high activity and low reaction energy barrier in catalytic hydroxylation of benzene at room temperature. These findings provide a route to controllably produce stable single-metal site catalysts and an engineering approach for regulating the central metal to improve catalytic performance.

中文翻译：

阳离子交换诱导单铜位点的精确调控触发苯的室温氧化

具有高催化活性和选择性的预期配位环境的稳定单金属位点催化剂的可控合成仍然具有挑战性。在这里，我们提出了一种阳离子交换策略，用于精确生产富边缘的硫 (S) 和氮 (N) 双修饰的单金属 (M) 位点催化剂（M = Cu、Pt、Pd 等）库. 我们的策略依赖于硫化物的阴离子骨架和富含 N 的聚合物壳在高温退火过程中产生大量的 S 和 N 缺陷，进一步促进具有原子分散性和优异可及性的交换金属物种的稳定。这个过程是通过原位透射电子显微镜追踪的，在此期间没有观察到金属聚集体。实验和理论结果都揭示了精确获得的 S，N双修饰的Cu位点在室温催化苯羟基化中表现出高活性和低反应能垒。这些发现为可控地生产稳定的单金属位点催化剂和调节中心金属以提高催化性能提供了一种工程方法。

更新日期：2020-06-25

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