期刊
JOURNAL OF CLEANER PRODUCTION
卷 384, 期 -, 页码 -出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.jclepro.2022.135509
关键词
Metal-organic frameworks; ?OH radical; Oxidative desulfurization; Pyrolysis; Vanadium nitride
Vanadium nitride was successfully used in the oxidative desulfurization of liquid fuel, with carbon-supported vanadium nitride (VN@C) prepared from pyrolysis of urea-loaded MOF. The VN@C(1100) catalyst prepared at 1100 degrees C showed the highest turnover frequency and low activation energy among reported vanadium-based catalysts. Experimental and theoretical studies confirmed the beneficial role of VN in the adsorption and activation of H2O2 to form •OH radical. The VN@C(1100) catalyst exhibited good stability after five cycles.
Vanadium nitride was firstly applied to oxidative desulfurization (ODS) of liquid fuel. Carbon-supported vana-dium nitride (VN@C) was prepared from pyrolysis of urea-loaded MOF, MIL-100(V), especially in the absence of external ammonia flow. One catalyst prepared at 1100 degrees C, VN@C(1100), had the highest turnover frequency of 18.8 h- 1 (with a very low activation energy of 29.9 kJmol-1) among the reported vanadium-based catalysts. The ESR and scavenger experiments confirmed center dot OH radical was the active species for the ODS. Calculations using density functional theory could support the beneficial role of VN (compared with conventional oxides) both in the adsorption of H2O2 and center dot OH and H2O2 activation to form center dot OH radical. The VN@C(1100) catalyst could be used for five cycles without any loss in activity. Therefore, supported vanadium nitrides could be suggested as a potential catalyst for oxidations that use H2O2 as an oxidant. Moreover, supported vanadium nitrides could be facilely derived from the pyrolysis of urea-loaded V-based MOFs, without ammonia flow.
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