Defect Pyrochlore‐Type Mott–Schottky Photocatalysts for Enhanced Ammonia Synthesis at Low Pressure

The ambient ammonia synthesis coupled with distributed green hydrogen production technology can provide promising solutions for low‐carbon NH3 production and H2 storage. Herein, we reported Ru‐loaded defective pyrochlore K2Ta2O6−x with remarkable visible‐light absorption and a very low work function...

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Veröffentlicht in:Angewandte Chemie International Edition 2023-06, Vol.62 (26), p.e202303629-n/a
Hauptverfasser: Zhao, Zihan, Tan, Ruike, Kong, Yuxiang, Zhang, Zihao, Qiu, Shou, Mu, Xiaoyue, Li, Lu
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Sprache:eng
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Zusammenfassung:The ambient ammonia synthesis coupled with distributed green hydrogen production technology can provide promising solutions for low‐carbon NH3 production and H2 storage. Herein, we reported Ru‐loaded defective pyrochlore K2Ta2O6−x with remarkable visible‐light absorption and a very low work function, enabling effective visible‐light‐driven ammonia synthesis from N2 and H2 at low pressure down to 0.2 atm. The photocatalytic rate was 2.8 times higher than that of the best previously reported photocatalyst and the photo‐thermal rate at 425 K was similar to that of Ru‐loaded black TiO2 at 633 K. Compared to perovskite‐type KTaO3−x with the same composition, the pyrochlore exhibited a 3.7‐fold increase in intrinsic activity due to a higher photoexcited charge separation efficiency and a higher conduction band position. The interfacial Schottky barrier and spontaneous electron transfer between K2Ta2O6−x and Ru further improve photoexcited charge separation and accumulate energetic electrons to facilitate N2 activation. Ru‐loaded defective pyrochlore K2Ta2O6−x was synthesized with visible light absorption and extremely low work function. High‐efficiency photocatalytic ammonia synthesis was achieved at low pressure with excellent catalytic activities. The pyrochlore structure exhibits amazing intrinsic activity, markedly enhances N2 dissociation on Ru, and is expected to be an ideal material for efficient ambient ammonia synthesis.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202303629