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 | Zhang, Ting1; Zhang, Di1; Han, Xinghua2; Dong, Ting2; Guo, Xinwen1; Song, Chunshan1,3,4; Si, Rui5; Liu, Wei6; Liu, Yuefeng6; Zhao, Zhongkui1 |
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 |
DOI | 10.1021/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 |
WOS研究方向 | Chemistry |
WOS类目 | Chemistry, Multidisciplinary |
语种 | 英语 |
出版者 | AMER CHEMICAL SOC |
WOS记录号 | WOS:000453488500014 |
URI标识 | http://www.irgrid.ac.cn/handle/1471x/2372948 |
专题 | 大连化学物理研究所 |
通讯作者 | Si, Rui; Liu, Yuefeng; Zhao, Zhongkui |
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 | 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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来源:大连化学物理研究所
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