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Preassembly Strategy To Fabricate Porous Hollow Carbonitride Spheres Inlaid with Single Cu-N-3 Sites for Selective Oxidation of Benzene to Phenol

文献类型：期刊论文

作者Dong, Ting2; Song, Chunshan1,3,4; Zhao, Zhongkui1; Liu, Wei6; Si, Rui5; Liu, Yuefeng6; Zhang, Ting1; Zhang, Di1; Han, Xinghua2; Guo, Xinwen1
刊名JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
出版日期2018-12-12
卷号140期号:49页码:16936-16940
ISSN号0002-7863
DOI10.1021/jacs.8b10703
通讯作者Si, Rui(sirui@sinap.ac.cn) ; Liu, Yuefeng(yuefeng.liu@dicp.ac.cn) ; Zhao, Zhongkui(zkzhao@dlut.edu.cn)
英文摘要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-N-3 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-N-3 sites in the porous hollow structure. An 86% conversion of benzene, with an unexpectedly high phenol selectivity of 96.7% at 60 degrees 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.
WOS关键词METAL-ORGANIC FRAMEWORKS ; ATOM CATALYST ; NITRIDE ; COMPLEXES ; OXYGEN ; PHOTOCATALYSTS ; HYDROGENATION ; HYDROXYLATION ; CLUSTERS ; METHANOL
资助项目National Natural Science Foundation of China[U1610104] ; National Natural Science Foundation of China[21676046]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000453488500014
出版者AMER CHEMICAL SOC
资助机构National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China
源URL[http://cas-ir.dicp.ac.cn/handle/321008/166370]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Zhao, Zhongkui; Si, Rui; Liu, Yuefeng
作者单位1.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian 116024, Peoples R China
2.North Univ China, Sch Chem Engn & Technol, Taiyuan 030051, Peoples R China
3.Penn State Univ, PSU DUT Joint Ctr Energy Res, EMS Energy Inst, University Pk, PA 16802 USA
4.Penn State Univ, Dept Energy & Mineral Engn & Chem Engn, University Pk, PA 16802 USA
5.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
6.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
推荐引用方式
GB/T 7714		 Dong, Ting,Song, Chunshan,Zhao, Zhongkui,et al. Preassembly Strategy To Fabricate Porous Hollow Carbonitride Spheres Inlaid with Single Cu-N-3 Sites for Selective Oxidation of Benzene to Phenol[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2018,140(49):16936-16940.
APA Dong, Ting.,Song, Chunshan.,Zhao, Zhongkui.,Liu, Wei.,Si, Rui.,...&Guo, Xinwen.(2018).Preassembly Strategy To Fabricate Porous Hollow Carbonitride Spheres Inlaid with Single Cu-N-3 Sites for Selective Oxidation of Benzene to Phenol.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,140(49),16936-16940.
MLA Dong, Ting,et al."Preassembly Strategy To Fabricate Porous Hollow Carbonitride Spheres Inlaid with Single Cu-N-3 Sites for Selective Oxidation of Benzene to Phenol".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 140.49(2018):16936-16940.

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来源：大连化学物理研究所

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