Atomically Dispersed Co-P-3 on CdS Nanorods with Electron-Rich Feature Boosts Photocatalysis
Author(s)
Zhou, Peng
Zhang, Qinghua
Xu, Zhikun
Shang, Qiuyu
Wang, Liang
Chao, Yuguang
Li, Yiju
Chen, Hui
Lv, Fan
Zhang, Qing
Gu, Lin
Guo, Shaojun
Griffith University Author(s)
Year published
2019
Metadata
Show full item recordAbstract
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 ...
View more >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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View more >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.
View less >
Journal Title
Advanced Materials
Volume
32
Issue
7
Subject
Physical sciences
Chemical sciences
Engineering
Science & Technology
Chemistry, Multidisciplinary
Chemistry, Physical