Graphene Quantum Sheet Catalyzed Silicon Photocathode for Selective CO 2 Conversion to CO

Graphene Quantum Sheet Catalyzed Silicon Photocathode for Selective CO 2 Conversion to CO
graphene; CO2 reduction; silicon; photocatalyst
Issue Date
Advanced functional materials
The reduction of carbon dioxide (CO 2 ) into chemical feedstock is drawing increasing attention as a prominent method of recycling atmospheric CO 2 . Although many studies have been devoted in designing an effi cient catalyst for CO 2 conversion with noble metals, low selectivity and high energy input still remain major hurdles. One possible solution is to use the combination of an earth-abundant electrocatalyst with a photoelectrode powered by solar energy. Herein, for the fi rst time, a p-type silicon nanowire with nitrogen-doped graphene quantum sheets (N-GQSs) as heterogeneous electrocatalyst for selective CO production is demonstrated. The photoreduction of CO 2 into CO is achieved at a potential of −1.53 V versus Ag/Ag + , providing 0.15 mA cm −2 of current density, which is 130 mV higher than that of a p-type Si nanowire decorated with well-known Cu catalyst. The faradaic effi ciency for CO is 95%, demonstrating signifi cantly improved selectivity compared with that of bare planar Si. The density functional theory (DFT) calculations are performed, which suggest that pyridinic N acts as the active site and band alignment can be achieved for N-GQSs larger than 3 nm. The demonstrated high efficiency of the catalytic system provides new insights for the development of nonprecious, environmentally benign CO 2 utilization.
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