Journal
ENERGY & FUELS
Volume 35, Issue 23, Pages 19185-19190Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.energyfuels.1c02819
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Funding
- National Key Research and Development Program of China [2017YFA0206903]
- National Natural Science Foundation of China [22088102, 21861132004, 21971251]
- Strategic Priority Research Program of Chinese Academy of Science [XDB17000000]
- Youth Innovation Promotion Association of Chinese Academy of Sciences [2018031]
- Chinese Academy of Sciences (CAS) Project for Young Scientists in Basic Research [YSBR-004]
- Key Research Program of Frontier Science of Chinese Academy of Sciences [QYZDYSSW-JSC029]
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The study revealed the in situ binding form between QDs and Ni2+ salts in a high-efficiency H-2 evolution photosystem, demonstrating that Ni-0 clusters formed in situ on the surface of QDs via a Ni-S bond act as the real catalytic species for H-2 photogeneration.
Artificial photosystems consisting of colloidal semiconductor quantum dots (QDs) and non-noble metal salts (e.g., Ni2+) show exceptional photocatalytic H-2 activity. Recent studies have found the structure of the catalysts distorted during the photocatalytic H-2 evolution reaction, which significantly influences the reaction kinetics. However, the in situ binding form between QDs and the catalytic center is still ambiguous. Herein, we reveal that, in the high-efficiency H-2 evolution photosystem based on CdS-S2- QDs and water-soluble Ni2+ salts (pH 6.0), the Ni-0 clusters formed in situ bind on the surface of QDs via a Ni-S bond to work as the real catalytic species for H-2 photogeneration, manifested by a combination of X-ray photoelectron spectroscopy, electron paramagnetic resonance, X-ray absorption spectroscopy, and a set of control experiments.
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