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

Ting Zhang, Di Zhang, Xinghua Han, Ting Dong, Xinwen Guo, Chunshan Song, Rui Si, Wei Liu, Yuefeng Liu, Zhongkui Zhao

Research output: Contribution to journalArticle

5 Citations (Scopus)

Abstract

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 °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.

Original languageEnglish (US)
Pages (from-to)16936-16940
Number of pages5
JournalJournal of the American Chemical Society
Volume140
Issue number49
DOIs
StatePublished - Dec 12 2018

Fingerprint

Carbon nitride
Phenol
Benzene
Phenols
Atoms
Oxidation
Extended X ray absorption fine structure spectroscopy
Catalysts
Melamine
Nanostructures
Aberrations
Polymerization
Nanoparticles
Electron microscopy
Catalytic Domain
Spectrum Analysis
Electron Microscopy
Hot Temperature
X-Rays
Temperature

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Zhang, Ting ; Zhang, Di ; Han, Xinghua ; Dong, Ting ; Guo, Xinwen ; Song, Chunshan ; Si, Rui ; Liu, Wei ; Liu, Yuefeng ; Zhao, Zhongkui. / Preassembly Strategy to Fabricate Porous Hollow Carbonitride Spheres Inlaid with Single Cu-N 3 Sites for Selective Oxidation of Benzene to Phenol In: Journal of the American Chemical Society. 2018 ; Vol. 140, No. 49. pp. 16936-16940.
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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, Ting; Zhang, Di; Han, Xinghua; Dong, Ting; Guo, Xinwen; Song, Chunshan; Si, Rui; Liu, Wei; Liu, Yuefeng; Zhao, Zhongkui.

In: Journal of the American Chemical Society, Vol. 140, No. 49, 12.12.2018, p. 16936-16940.

Research output: Contribution to journalArticle

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AU - Zhang, Di

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AU - Guo, Xinwen

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AU - Si, Rui

AU - Liu, Wei

AU - Liu, Yuefeng

AU - Zhao, Zhongkui

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