Oxidative denitrogenation of liquid fuel over W2N@carbon catalyst derived from a phosphotungstinic acid encapsulated metal–azolate framework

Biswa Nath Bhadra, Yong Su Baek, Sunghwan Kim, Cheol Ho Choi, Sung Hwa Jhung

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44 Scopus citations

Abstract

Tungsten nitride-incorporated carbon (W2N(x)@C) was firstly prepared via pyrolysis of a newly developed phosphotungstic acid-loaded metal-azolate framework-6, PTA(x)@MAF-6 s. The obtained (without ammonia feeding) W2N(x)@C materials, were utilized as catalysts for oxidative denitrogenation (ODN) of fuels. The W2N(x)@C materials, especially W2N(15)@C, under ultrasound (US) irradiation was found to be a very efficient catalyst for oxidative removal of various organo-nitrogen compounds (ONCs). Importantly, the W2N(15)@C showed around 80–147 times turnover frequency those of reported catalysts for stubborn carbazole oxidation. Electron density on the N-atom of the ONCs has a dominant role in the oxidation. The oxidation mechanism was suggested mainly based on the calculated electron density of the reactants and analysis of major intermediates/products. Moreover, the US-assisted ODN was progressed by both non-radical and radical paths, as supported by the electron spin resonance and radical scavenger experiments. The recyclability of the catalyst in the US irradiative ODN was also confirmed.

Original languageEnglish
Article number119842
JournalApplied Catalysis B: Environmental
Volume285
DOIs
StatePublished - 15 May 2021

Keywords

  • Denitrogenation
  • Organo-nitrogen compounds
  • Oxidation
  • Tungsten nitride
  • Ultrasound

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