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

doi:10.1021/jacs.8b10703

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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, T ; Zhang, D ; Han, XH ; Dong, T ; Guo, XW ; Song, CS ; Si, R ; Liu, W ; Liu, YF ; Zhao, ZK
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2018
卷号	140 期号:49 页码:16936-16940
关键词	METAL-ORGANIC FRAMEWORKS ATOM CATALYST NITRIDE COMPLEXES OXYGEN PHOTOCATALYSTS HYDROGENATION HYDROXYLATION CLUSTERS METHANOL
ISSN号	0002-7863
DOI	10.1021/jacs.8b10703
文献子类	期刊论文
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.
语种	英语
内容类型	期刊论文
源URL	[http://ir.sinap.ac.cn/handle/331007/31064]
专题	上海应用物理研究所_中科院上海应用物理研究所2011-2017年
作者单位	1.Penn State Univ, Dept Energy & Mineral Engn & Chem Engn, University Pk, PA 16802 USA 2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 3.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian 116024, Peoples R China 4.North Univ China, Sch Chem Engn & Technol, Taiyuan 030051, Peoples R China 5.Penn State Univ, PSU DUT Joint Ctr Energy Res, EMS Energy Inst, University Pk, PA 16802 USA 6.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
推荐引用方式 GB/T 7714	Zhang, T,Zhang, D,Han, XH,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, T.,Zhang, D.,Han, XH.,Dong, T.,Guo, XW.,...&Zhao, ZK.(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, T,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.