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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
Zhang, Ting1; Zhang, Di1; Han, Xinghua2; Dong, Ting2; Guo, Xinwen1; Song, Chunshan1,3,4; Si, Rui5; Liu, Wei6; Liu, Yuefeng6; Zhao, Zhongkui1
Corresponding AuthorSi, Rui(sirui@sinap.ac.cn) ; Liu, Yuefeng(yuefeng.liu@dicp.ac.cn) ; Zhao, Zhongkui(zkzhao@dlut.edu.cn)
Source PublicationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2018-12-12
ISSN0002-7863
DOI10.1021/jacs.8b10703
Volume140Issue:49Pages:16936-16940
Funding ProjectNational Natural Science Foundation of China[U1610104] ; National Natural Science Foundation of China[21676046]
Funding OrganizationNational 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
WOS SubjectChemistry, Multidisciplinary
WOS Research AreaChemistry
WOS KeywordMETAL-ORGANIC FRAMEWORKS ; ATOM CATALYST ; NITRIDE ; COMPLEXES ; OXYGEN ; PHOTOCATALYSTS ; HYDROGENATION ; HYDROXYLATION ; CLUSTERS ; METHANOL
AbstractDeveloping 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.
Language英语
Funding OrganizationNational 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
WOS IDWOS:000453488500014
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:2[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/166371
Collection中国科学院大连化学物理研究所
Corresponding AuthorSi, Rui; Liu, Yuefeng; Zhao, Zhongkui
Affiliation1.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
Recommended Citation
GB/T 7714
Zhang, Ting,Zhang, Di,Han, Xinghua,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 Zhang, Ting.,Zhang, Di.,Han, Xinghua.,Dong, Ting.,Guo, Xinwen.,...&Zhao, Zhongkui.(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 Zhang, 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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