Abstract
Although the enhanced intrinsic activities of some nano-metal oxides are obtained by manufacturing oxygen vacancies (OVs), the effect of multiple roles of OVs is ambiguous. Herein, an interface catalytic regulation via electron rearrangement and hydroxyl radicals (˙OH) was proposed with the designed ZrO(2) hollow sphere rich in OVs (V(o)-rich ZrO(2)). Surprisingly, it was shown that the catalytic ability of V(o)-rich ZrO(2) was 9.9 times higher than that of ZrO(2) with little OVs in electrochemical catalytic reduction of Pb(ii). It was found that the generation of Zr(2+) and Zr(3+) caused by OVs results in the rearrangement of abundant free electrons to facilitate the catalytic reaction rates. The longer bond length between V(o)-rich ZrO(2) and reactants, and the lower adsorption energy are beneficial for reactants to desorb, improving the conversion rates. Besides, the produced ˙OH were captured which were induced by OVs and trace divalent heavy metal ions in in situ electron paramagnetic resonance (EPR) experiments, contributing to lowering the energy barriers. This study not only revealed the enhanced interface catalytic effect of electron rearrangement and generated ˙OH triggered by OVs, but also provided unique insights into interface catalytic regulation on nano-metal oxides simulated by OVs.