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- W4316505596 abstract "Photoelectrochemistry that directly takes advantage of solar energy by photoelectrodes is a promising green route for the nitrogen fixation, but is currently far from practical application. It is necessary to understand the structure-reactivity interplay of the photocathodes for rendering rational improvement of the existing challenges. Here, we make efforts to reveal AuCoPd-CoOx/SiO2/Si photocathodes capable of selective photoelectrochemical conversion of nitrogen to ammonia at varied pressures, achieving an ammonia yield rate of 22.2 ± 0.4 μg·h−1·cm−2 and a faradic efficiency of 22.9% at −0.1 V vs. reversible hydrogen electrode under 3-MPa nitrogen. In particular, we focus on the remarkable, but often subtle, roles of the synergy between electron localization and alloying in determining the reactivity of the photocathodes. Specifically, operando XPS and XAS illustrate that the oxidation states of Au and Pd enable the photoinduced electron capture as the reduction sites to produce the *N2 and *H active species, respectively, facilitating the couple of N-H for ammonia synthesis. Although this study is not sufficient to break through bottleneck, there is much insight on the design of efficient and robust photocathodes for photoelectrochemical nitrogen fixation." @default.
- W4316505596 created "2023-01-16" @default.
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- W4316505596 date "2023-02-01" @default.
- W4316505596 modified "2023-10-14" @default.
- W4316505596 title "Deciphering the synergy between electron localization and alloying for photoelectrochemical nitrogen reduction to ammonia" @default.
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- W4316505596 doi "https://doi.org/10.1016/s1872-2067(22)64178-0" @default.
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