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d-Band Center Engineering of BiVO4 Photoanode for Boosting Bilateral Synergistic Interface Toward Efficient Photoelectrocatalytic CO2 Reduction With BiCu Cathode
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DOI：10.1002/cssc.70956.png)
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Abstract
En 中文
Photoelectrocatalytic (PEC) CO2 reduction offers a sustainable route to address energy and environmental challenges. Herein, we designed a photoanode–cathode cooperative strategy by coupling d-band center-regulated BiVO4 photoanodes (t/m-BiVO4, m-BiVO4, and m-BiVO4/Bi) with a BiCu cathode to elucidate bilateral synergy in PEC CO2 reduction. Among the evaluated photoanodes, the m-BiVO4/Bi delivers superior photoelectrochemical performance, achieving 98.84% Faradaic efficiency toward quantified liquid products, an applied-bias photon-to-current efficiency of 1.67% at 0.6 V versus reversible hydrogen electrode (RHE), and a photocurrent density of 5.59 mA·cm−2 at 1.23 V versus RHE. More importantly, the CO2 reduction pathways are tunable. In particular, the m-BiVO4/Bi‖BiCu favors the C2 pathway (HCOOH → C2H5OH) over −0.7 to −1.1 V versus RHE. The improved performance is attributed to an optimized photoanode electronic structure that facilitates hole injection to accelerate water-oxidation kinetics, thereby supplying an optimal proton–electron flux to the cathode, boosting overall PEC activity, and creating favorable conditions conducive to C─C coupling. This work highlights photoanode electronic-structure engineering as an effective lever to modulate the product selectivity and interfacial reaction dynamics in PEC CO2 reduction.
Keywords:
Bi-based materials
CO2 reduction
d-band center
photoanode
photoelectrocatalysis
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