Encapsulation of HPW and preparation of composites rich in Zr-defects by manual grinding: Synergistic catalysis for efficient oxidative desulfurization at room temperature

The development of catalysts with excellent performance in oxidative desulfurization (ODS) at room temperature will greatly facilitate the advancement of desulfurization technology. An efficient novel strategy, 4-aminopyridine molecular bridging combined with manual grinding, was presented to encapsulate HPW into UiO-66 for achieving stable loading of PW and to produce abundant defects that contribute to the formation of active complexes with strong oxidation ability. The prepared catalyst showed outstanding catalytic activity in the ODS system, achieving full desulfurization in 15 min at room temperature and a low O/S molar ratio. Further investigations reveal that the synergistic catalytic effect of the faulty UiO-66 and PW is mostly responsible for superior catalytic performance. UiO-66 rich in defects promote the decomposition of H2O2 into radicals, and PW can combine with the radicals to form more stable active peroxide intermediates, then exerting the catalytic ability of ODS at room temperature. Such a synergistic catalytic mechanism provides a guide to improving the oxidation ability of PW-based catalysts at room temperature.