4.8 Article

Boron-doped melamine-derived carbon nitrides tailored by ionic liquids for catalytic conversion of CO2 into cyclic carbonates

Journal

GREEN CHEMISTRY
Volume 19, Issue 13, Pages 2957-2965

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c7gc00279c

Keywords

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Funding

  1. National Key Projects for Fundamental Research and Development of China [2016YFB0600903]
  2. National Natural Science Foundation of China [21676274]
  3. Key Program of National Natural Science Foundation of China [91434203]
  4. Key Research Program of Frontier Sciences, CAS [QYZDY-SSW-JSC011]
  5. Fund of State Key Laboratory of Multiphase Complex Systems, IPE, CAS [MPCS-2015-A-05]

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A new approach to tailoring edge active groups of graphitic carbon nitrides for catalytic conversion of CO2 into cyclic carbonates was proposed in this work. To improve the catalytic performance, boron-doped melamine-derived graphitic carbon nitrides (MCNB) with numerous exposed edge defects were prepared by using 1-butyl-3-methylimidazolium tetrafluoroborate (BmimBF(4)) as the soft template and boron source. Different mass ratios of BmimBF(4) to melamine were explored for MCNB preparation, MCNB(x) (x is the mass ratio) with different polymerization degree, pore structure and boron doping content were obtained, and the relationship between MCNB properties and the corresponding catalytic activity was then investigated. With low polymerization degree, abundant meso-macroporous structure and small amounts of boron (<1.59 atm%) doped in the skeleton, MCNB(0.01) exhibited better catalytic performance and could be suitable for various epoxide substrates with the yield of cyclic carbonates up to 89.0% at 130 degrees C in 6 h. According to the XPS analysis and DFT calculation results, the active centers were confirmed to be the partially-condensed amino groups in edge defects, which were enhanced by moderate doping of boron in the skeleton.

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