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Iced photochemical reduction to synthesize atomically dispersed metals by suppressing nanocrystal growth.

ABSTRACT: Photochemical solution-phase reactions have been widely applied for the syntheses of nanocrystals. In particular, tuning of the nucleation and growth of solids has been a major area of focus. Here we demonstrate a facile approach to generate atomically dispersed platinum via photochemical reduction of frozen chloroplatinic acid solution using ultraviolet light. Using this iced-photochemical reduction, the aggregation of atoms is prevented, and single atoms are successfully stabilized. The platinum atoms are deposited on various substrates, including mesoporous carbon, graphene, carbon nanotubes, titanium dioxide nanoparticles, and zinc oxide nanowires. The atomically dispersed platinum on mesoporous carbon exhibits efficient catalytic activity for the electrochemical hydrogen evolution reaction, with an overpotential of only 65?mV at a current density of 100?mA?cm^-2 and long-time durability (>10?h), superior to state-of-the-art platinum/carbon. This iced-photochemical reduction may be extended to other single atoms, for example gold and silver, as demonstrated in this study.

SUBMITTER: Wei H

PROVIDER: S-EPMC5684195 | biostudies-literature | 2017 Nov

REPOSITORIES: biostudies-literature

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Iced photochemical reduction to synthesize atomically dispersed metals by suppressing nanocrystal growth.

Wei Hehe H Huang Kai K Wang Da D Zhang Ruoyu R Ge Binghui B Ma Jingyuan J Wen Bo B Zhang Shuai S Li Qunyang Q Lei Ming M Zhang Cheng C Irawan Joshua J Liu Li-Min LM Wu Hui H

Nature communications 20171114 1

Photochemical solution-phase reactions have been widely applied for the syntheses of nanocrystals. In particular, tuning of the nucleation and growth of solids has been a major area of focus. Here we demonstrate a facile approach to generate atomically dispersed platinum via photochemical reduction of frozen chloroplatinic acid solution using ultraviolet light. Using this iced-photochemical reduction, the aggregation of atoms is prevented, and single atoms are successfully stabilized. The platin ...[more]

PMID: 29133795

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Project description:Highlights Fe single atoms supported on porous carbon nanofiber are prepared by spatial confinement. The iron single atoms supported on porous nitrogen-doped carbon nanofibers (FeSAs-NCF) can promote the reversible conversion between aluminum polysulfides. The FeSAs-NCF can chemically anchor the polysulfides to suppress shuttle effect. Supplementary Information The online version contains supplementary material available at 10.1007/s40820-022-00915-4. Rechargeable aluminum–sulfur (Al–S) batteries have been considered as a highly potential energy storage system owing to the high theoretical capacity, good safety, abundant natural reserves, and low cost of Al and S. However, the research progress of Al–S batteries is limited by the slow kinetics and shuttle effect of soluble polysulfides intermediates. Herein, an interconnected free-standing interlayer of iron single atoms supported on porous nitrogen-doped carbon nanofibers (FeSAs-NCF) on the separator is developed and used as both catalyst and chemical barrier for Al–S batteries. The atomically dispersed iron active sites (Fe–N4) are clearly identified by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption near-edge structure. The Al–S battery with the FeSAs-NCF shows an improved specific capacity of 780 mAh g−1 and enhanced cycle stability. As evidenced by experimental and theoretical results, the atomically dispersed iron active centers on the separator can chemically adsorb the polysulfides and accelerate reaction kinetics to inhibit the shuttle effect and promote the reversible conversion between aluminum polysulfides, thus improving the electrochemical performance of the Al–S battery. This work provides a new way that can not only promote the conversion of aluminum sulfides but also suppress the shuttle effect in Al–S batteries. Supplementary Information The online version contains supplementary material available at 10.1007/s40820-022-00915-4.

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Iced photochemical reduction to synthesize atomically dispersed metals by suppressing nanocrystal growth.

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Iced photochemical reduction to synthesize atomically dispersed metals by suppressing nanocrystal growth.

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