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J Am Chem Soc. 2018 Dec 12;140(49):16936-16940. doi: 10.1021/jacs.8b10703. Epub 2018 Dec 3.

Preassembly Strategy To Fabricate Porous Hollow Carbonitride Spheres Inlaid with Single Cu-N3 Sites for Selective Oxidation of Benzene to Phenol.

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State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering , Dalian University of Technology , Dalian 116024 , P. R. China.
School of Chemical Engineering and Technology , North University of China , Taiyuan 030051 , P. R. China.
EMS Energy Institute, PSU-DUT Joint Center for Energy Research and Department of Energy & Mineral Engineering and Chemical Engineering , Pennsylvania State University , University Park , Pennsylvania 16802 , United States.
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics , Chinese Academy of Sciences , Shanghai 201204 , P.R. China.
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics , Chinese Academy of Sciences , Dalian 116023 , P. R. China.


Developing single-atom catalysts with porous micro-/nanostructures for high active-site accessibility is of great significance but still remains a challenge. Herein, we for the first time report a novel template-free preassembly strategy to fabricate porous hollow graphitic carbonitride spheres with single Cu atoms mounted via thermal polymerization of supramolecular preassemblies composed of a melamine-Cu complex and cyanuric acid. Atomically dispersed Cu-N3 moieties were unambiguously confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure spectroscopy. More importantly, this material exhibits outstanding catalytic performance for selective oxidation of benzene to phenol at room temperature, especially showing phenol selectivity (90.6 vs 64.2%) and stability much higher than those of the supported Cu nanoparticles alone, originating from the isolated unique Cu-N3 sites in the porous hollow structure. An 86% conversion of benzene, with an unexpectedly high phenol selectivity of 96.7% at 60 °C for 12 h, has been achieved, suggesting a great potential for practical applications. This work paves a new way to fabricate a variety of single-atom catalysts with diverse graphitic carbonitride architectures.


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