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

18 Scopus citations

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

All Science Journal Classification (ASJC) codes

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

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