Atomically Dispersed Co-P3 on CdS Nanorods with Electron-Rich Feature Boosts Photocatalysis
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 32(2020), 7 vom: 24. Feb., Seite e1904249 |
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1. Verfasser: | |
Weitere Verfasser: | , , , , , , , , , , |
Format: | Online-Aufsatz |
Sprache: | English |
Veröffentlicht: |
2020
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Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
Schlagworte: | Journal Article Co single atoms formic acid dehydrogenation non-noble metal catalysts phosphorus coordination photocatalysis |
Zusammenfassung: | © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. The development of highly efficient photocatalytic systems with rapid photogenerated charge separation and high surface catalytic activity is highly desirable for the storage and conversion of solar energy, yet remains a grand challenge. Herein, a conceptionally new form of atomically dispersed Co-P3 species on CdS nanorods (CoPSA-CdS) is designed and synthesized for achieving unprecedented photocatalytic activity for the dehydrogenation of formic acid (FA) to hydrogen. X-ray absorption near edge structure, X-ray photoelectron spectroscopy, and time-resolved photoluminescence results confirm that the Co-P3 species have a unique electron-rich feature, greatly improving the efficiency of photogenerated charge separation through an interface charge effect. The in situ attenuated total reflection infrared spectra reveal that the Co-P3 species can achieve much better dissociation adsorption of FA and activation of CH bonds than traditional sulfur-coordinated Co single atom-loaded CdS nanorods (CoSSA-CdS). These two new features make CoPSA-CdS exhibit the unprecedented 50-fold higher activity in the photocatalytic dehydrogenation of FA than CoSSA-CdS, and also much better activity than the Ru-, Rh-, Pd-, or Pt-loaded CdS. Besides, CoPSA-CdS also shows the highest mass activity (34309 mmol gCo -1 h-1 ) of Co reported to date. First-principles simulation reveals that the Co-P3 species herein can form an active PHCOO intermediate for enhancing the rate-determining dissociation adsorption of FA |
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Beschreibung: | Date Revised 30.09.2020 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.201904249 |