Oxidative desulfurization (ODS) has been a promising technology for removing sulfur compounds from fuel oil under mild conditions. It is essential to design ODS catalyst exposing plentiful accessible active sites, but it remains a challenge. Here, we have reported the design of cluster-like Mo2N catalyst (1.5 nm) uniformly dispersed on graphene surface by anchoring PMo12 polyoxometalate clusters on polyethyleneimine (PEI)-modified graphite oxide (GO). The obtained Mo2N/rGO-A catalyst has highly exposed active sites and plentiful accessible surface. Importantly, Mo2N catalyst can readily activate oxidant to generate active Mo2N-peroxo intermediates. In the ODS reaction of dibenzothiophene (DBT) with H2O2 as the oxidant, the catalyst can achieve the complete removal of sulfur compounds (1000 ppm) within 15 min, with a reaction rate constant k of 1.94 × 10-1 min-1 at 60 °C, being superior to the corresponding Mo-O-based catalysts, large-sized Mo2N/rGO-D catalyst and the most of the reported transition metal-based catalysts. Furthermore, the catalyst shows good cycling stability with no obvious deactivation after eight cycles. The ODS reaction of DBT over Mo2N/rGO-A catalyst mainly follows a non-radical oxidation mechanism with DBTO2 (dibenzothiophene sulfone) being the only oxidation product based on the free radical scavenger experiment and GC-MS analysis. This work has important implications for the design of efficient and stable small-sized Mo-based catalyst for ODS of fuel oil.
Dielectric barrier discharge (DBD) plasma-assisted ammonia decomposition reaction was investigated to produce carbon-free hydrogen for fuel cell applications . Mo 2 N catalyst was synthesized and applied for catalytic ammonia decomposition in different reaction modes. The synergistic effect of using Mo 2 N catalyst in combination with DBD plasma resulted in near complete conversion of NH 3 decomposition at specific energy input (SEI) of 39.6 kJ L −1 , giving an energy efficiency of 6.1 mol·kWh −1 for H 2 production. The particle size of Mo 2 N catalyst was discovered to affect the plasma-catalytic performance for NH 3 decomposition, with Mo 2 N-powder catalyst showing higher reactivity compared with Mo 2 N-particle catalyst. The plasma diagnostic results showed that, compared to the filamentary discharge with Mo 2 N-particle catalyst, the Mo 2 N-powder catalyst packing lead to a predominant surface discharge; such localized surface discharges might contribute to a facile transportation of reactive species from the plasma phase to the catalyst surface , thus leading to higher plasma-catalytic performance.
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