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Water photosplitting: Atomistic mechanism and quantum dynamics
Author(s) -
Yutian Shen,
Sheng Meng
Publication year - 2019
Publication title -
wuli xuebao
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.199
H-Index - 47
ISSN - 1000-3290
DOI - 10.7498/aps.68.20181312
Subject(s) - water splitting , chemical physics , plasmon , antibonding molecular orbital , ultrashort pulse , electron transfer , molecular dynamics , plasmonic nanoparticles , materials science , physics , electron , nanotechnology , atomic physics , atomic orbital , photochemistry , chemistry , optoelectronics , photocatalysis , optics , laser , quantum mechanics , biochemistry , catalysis
Directly splitting water into carbon-free H 2 fuel and O 2 gases by sunlight is one of the most environmentally-friendly and potentially low cost approaches to solving the grand global energy challenge. Recent progress of electronic structure theory and quantum simulations allow us to directly explore the atomistic mechanism and ultrafast dynamics of water photosplitting on plasmonic nanoparticles. Here in this paper, we briefly introduce the relevant researches in our group. First we propose that the supported gold nanoparticles on oxide thin film/mental should be able to potentially serve as efficient photocatalysts for water splitting. Then, under the light illumination, we identify a strong correlation among light intensity, hot electron transfer rate, and water splitting reaction rate. The rate of water splitting is dependent not only on respective optical absorption strength, but also on the quantum oscillation mode of plasmonic excitation, which can help to design nanoparticles in water photosplitting cells. Finally, we simulate the ultrafast electron-nuclear quantum dynamics of H 2 generation with plasmonic gold cluster on a time scale of~100 fs in liquid water. We identify that the water splitting is dominated by field enhancement effect and associated with charge transfer from gold to antibonding orbital of water molecule. Based on all atomistic mechanism and quantum dynamics above, we present a “chain-reaction” H 2 production mechanism via high-speed (much higher than their thermal velocity) collision of two hydrogen atoms from different water molecules under light illumination.

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