Tailoring the Porosity in Iron Phosphosulfide Nanosheets to Improve the Performance of Photocatalytic Hydrogen Evolution

Metal sulfide photocatalysts are typically required during water splitting to produce hydrogen. However, the rapid recombination of photogenerated electron–hole pairs in these highly unstable photocatalysts has restricted hydrogen production to small‐scale batch reactions. In this work, porous trans...

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Bibliographic Details
Published in:ChemSusChem 2019-06, Vol.12 (12), p.2651-2659
Main Authors: Zhang, Jian, Feng, Fang, Pu, Yong, Li, Xing'ao, Lau, Cher Hon, Huang, Wei
Format: Article
Language:English
Subjects:
Acetaldehyde
Anions
FePS3
Hydrogen
Hydrogen evolution
Hydrogen production
Hydrogen-based energy
Nanocrystals
Nanosheets
Oxidation
Performance enhancement
Photocatalysis
Photocatalysts
Porosity
porous nanosheets
Reagents
stability
Stiffness
Structural stability
Triethylamine
Water splitting
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Summary:Metal sulfide photocatalysts are typically required during water splitting to produce hydrogen. However, the rapid recombination of photogenerated electron–hole pairs in these highly unstable photocatalysts has restricted hydrogen production to small‐scale batch reactions. In this work, porous transition‐metal thiophosphites were used to enable continuous long‐term hydrogen production through photocatalysis. A wide bandgap (2.04 eV) was essential for generating hydrogen at a rate of 305.6 μmol h−1 g−1, 180 % faster than nonporous FePS3 nanosheets. More importantly, the high in‐plane stiffness of these approximately 7 nm thick porous FePS3 nanosheets ensured structural stability during 56 h of continuous photocatalysis reactions. The reaction results with D2O instead of H2O indicated that hydrogen mainly came from H2O. Furthermore, a sacrificial reagent (triethylamine) was photodegraded into diethylamine and acetaldehyde through a monoelectronic oxidation process, as indicated by HPLC and LC–MS. This synthesis strategy reported for FePS3 porous nanosheets paves a new pathway for designing other dianion‐based inorganic nanocrystals for hydrogen energy applications. Get under the nanosheets! The porosity in iron phosphosulfide nanosheets can be tailored to improve the stability and efficiency of photocatalytic hydrogen evolution. Continuous long‐term hydrogen production was achieved owing to the wide bandgap (2.04 eV) and hydrogen was generated at a rate of 305.6 μmol h−1 g−1, which was 180 % faster than nonporous FePS3 nanosheets.
ISSN:1864-5631
1864-564X
DOI:10.1002/cssc.201900789