Rising local electron density of carbons for enhanced O2 activation at room temperature

Abstract

Room-temperature activation of O2 into super dioxide radical (O2•−) is a crucial step in oxidation processes. Here, the concept of tuning local electron density of carbons is adopted to develop highly efficient catalysts for molecular oxygen activation. We demonstrate that π electron of sp2 carbons is essential for activating O2 with assistance of ultra-micropore, and varying defects or functional groups yield local electron rearrangement of carbons with altering catalytic capacity. Bringing electron rich non-metallic doping can rise local electron intensity of modified carbons with improved oxygen activation. In addition, transition-metal-sp2-carbon nano-composites that readily surrender electrons are constructed, achieving O2•− formation without spatial confinement. Our findings provide fundamental insights into intrinsic mechanism of O2 activation and offer a general protocol to design and development of advanced carbon catalysts for low-temperature oxidations.