Boron-doped diamond semiconductor electrodes: Efficient photoelectrochemical CO2 reduction through surface modification

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Abstract

Competitive hydrogen evolution and multiple proton-coupled electron transfer reactions limit photoelectrochemical CO₂ reduction in aqueous electrolyte. Here, oxygen-terminated lightly boron-doped diamond (BDD_L) thin films were synthesized as a semiconductor electron source to accelerate CO₂ reduction. However, BDD_L alone could not stabilize the intermediates of CO₂ reduction, yielding a negligible amount of reduction products. Silver nanoparticles were then deposited on BDD_L because of their selective electrochemical CO₂ reduction ability. Excellent selectivity (estimated CO:H₂ mass ratio of 318:1) and recyclability (stable for five cycles of 3 h each) for photoelectrochemical CO₂ 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.

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