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Enhanced charge-carrier dynamics and efficient solar-to-urea conversion on Si-based photocathodes.


ABSTRACT: Photoelectrochemical (PEC) coupling of CO2 and nitrate can provide a useful and green source of urea, but the process is affected by the photocathodes with poor charge-carrier dynamics and low conversion efficiency. Here, a NiFe diatomic catalysts/TiO2 layer/nanostructured n+p-Si photocathode is rationally designed, achieving a good charge-separation efficiency of 78.8% and charge-injection efficiency of 56.9% in the process of PEC urea synthesis. Compared with the electrocatalytic urea synthesis by using the same catalysts, the Si-based photocathode shows a similar urea yield rate (81.1 mg·h-1·cm-2) with a higher faradic efficiency (24.2%, almost twice than the electrocatalysis) at a lower applied potential under 1 sun illumination, meaning that a lower energy-consumption method acquires more aimed productions. Integrating the PEC measurements and characterization results, the synergistic effect of hierarchical structure is the dominating factor for enhancing the charge-carrier separation, transfer, and injection by the matched band structure and favorable electron-migration channels. This work provides a direct and efficient route of solar-to-urea conversion.

SUBMITTER: Zhang X 

PROVIDER: S-EPMC10895350 | biostudies-literature | 2024 Feb

REPOSITORIES: biostudies-literature

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Enhanced charge-carrier dynamics and efficient solar-to-urea conversion on Si-based photocathodes.

Zhang Xiaoran X   Lyu Yanhong Y   Chen Chen C   Zheng Jianyun J   Jiang San Ping SP   Wang Shuangyin S  

Proceedings of the National Academy of Sciences of the United States of America 20240213 8


Photoelectrochemical (PEC) coupling of CO<sub>2</sub> and nitrate can provide a useful and green source of urea, but the process is affected by the photocathodes with poor charge-carrier dynamics and low conversion efficiency. Here, a NiFe diatomic catalysts/TiO<sub>2</sub> layer/nanostructured n<sup>+</sup>p-Si photocathode is rationally designed, achieving a good charge-separation efficiency of 78.8% and charge-injection efficiency of 56.9% in the process of PEC urea synthesis. Compared with t  ...[more]

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