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  • Title: Electron Delocalization Disentangles Activity-Selectivity Trade-Off of Transition Metal Phosphide Catalysts in Oxidative Desulfurization.
    Author: Zou J, Wu S, Lin Y, Li X, Niu Q, He S, Yang C.
    Journal: Environ Sci Technol; 2024 Aug 20; 58(33):14895-14905. PubMed ID: 39115177.
    Abstract:
    Breaking the activity-selectivity trade-off has been a long-standing challenge in catalysis. Here, we proposed a nanoheterostructure engineering strategy to overcome the trade-off in metal phosphide catalysts for the oxidative desulfurization (ODS) of fuels. Experimental and theoretical results demonstrated that electron delocalization was the key driver to simultaneously achieve high activity and high selectivity for the molybdenum phosphide (MoP)/tungsten phosphide (WP) nanoheterostructure catalyst. The electron delocalization not only promoted the catalytic pathway transition from predominant radicals to singlet oxygens in H2O2 activation but also simultaneously optimized the adsorption of reactants and intermediates on Mo and W sites. The presence of such dual-enhanced active sites ideally compensated for the loss of activity due to the nonradical catalytic pathway, consequently disentangling the activity-selectivity trade-off. The resulting catalyst (MoWP2/C) unprecedentedly achieved 100% removal of thiophenic compounds from real diesel at an initial concentration of 2676 ppm of sulfur with a high turnover frequency (TOF) of 105.4 h-1 and a minimal O/S ratio of 4. This work provides fundamental insight into the structure-activity-selectivity relationships of heterogeneous catalysts and may inspire the development of high-performance catalysts for ODS and other catalytic fields.
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