Boron-doped diamond semiconductor electrodes: Efficient photoelectrochemical CO 2 reduction through surface modification

Abstract

Competitive hydrogen evolution and multiple proton-coupled electron transfer reactions limit photoelectrochemical CO 2 reduction in aqueous electrolyte. Here, oxygen-terminated lightly boron-doped diamond (BDD L) thin films were synthesized as a semiconductor electron source to accelerate CO 2 reduction. However, BDD L alone could not stabilize the intermediates of CO 2 reduction, yielding a negligible amount of reduction products. Silver nanoparticles were then deposited on BDD L because of their selective electrochemical CO 2 reduction ability. Excellent selectivity (estimated CO:H 2 mass ratio of 318:1) and recyclability (stable for five cycles of 3 h each) for photoelectrochemical CO 2 reduction were obtained for the optimum silver nanoparticle-modified BDD L electrode at -1.1 V vs. RHE under 222-nm irradiation. The high efficiency and stability of this catalyst are ascribed to the in situ photoactivation of the BDD L surface during the photoelectrochemical reaction. The present work reveals the potential of BDD L as a high-energy electron source for use with co-catalysts in photochemical conversion.