Unique Dual-Sites Boosting Overall CO2 Photoconversion by Hierarchical Electron Harvesters

Low selectivity and poor activity of photocatalytic CO2 reduction process are usually limiting factors for its applicability. Herein, a hierarchical electron harvesting system is designed on Co-Ni-P hollow nano-millefeuille (Co-Ni-P NH), which enables the charge enrichment on Co-Ni dual active sites and selective conversion of CO2 to CH4. The Co-Ni-P serves as an electron harvester and photonic black hole accelerating the kinetics for CO2-catalyzed reactions. Moreover, the dual sites form from highly stable Co-O-Ni-C intermediates, which thermodynamically not only lower the reaction energy barrier but also transform the reaction pathways, thus enabling the highly selective generation of CH4 from CO2. As an outcome, the Co-Ni-P NH/black phosphorus with dual sites leads to a tremendously improved photocatalytic CH4 generation with a selectivity of 86.6% and an impressive activity of 38.7 mu mol g(-1) h(-1).

Automated summary

A hierarchical electron harvesting system was designed on Co-Ni-P hollow nano-millefeuille for selective conversion of CO2 to CH4, resulting in significantly improved photocatalytic CH4 generation with high selectivity.