Journal
NANO LETTERS
Volume 21, Issue 15, Pages 6449-6455Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c01187
Keywords
ab initio calculations; photocatalysis; graphitic carbon nitride; bond evolution; time dependent density functional theory
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Funding
- National Natural Science Foundation of China (NSFC) [12025407, 11974400, 11474328, 91850120]
- Ministry of Science and Technology of the People's Republic of China (MOST) [2016YFA0300902]
- CAS [XDB330301]
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In this study, a polymeric semiconductor-graphitic carbon nitride was chosen as a prototype substrate to investigate light-driven photocatalytic water splitting. The research reveals the transport channel of photogenerated charge carriers at the interface, proposes a three-step photoreaction mechanism, and presents insights for further development of efficient water-splitting photocatalysts from a dynamic perspective.
To elucidate the nature of light-driven photocatalytic water splitting, a polymeric semiconductor-graphitic carbon nitride (g-C3N4)-has been chosen as a prototype substrate for studying atomistic water spitting processes in realistic environments. Our nonadiabatic quantum dynamics simulations based on real-time time-dependent density functional theory reveal explicitly the transport channel of photogenerated charge carriers at the g-C3N4/water interface, which shows a strong correlation to bond re-forming. A three-step photoreaction mechanism is proposed, whereas the key roles of hole- driven hydrogen transfer and interfacial water configurations were identified. Immediately following photocatalytic water splitting, atomic pathways for the two dissociated hydrogen atoms approaching each other and forming the H-2 gas molecule are demonstrated, while the remanent OH radicals may form intermediate products (e.g., H2O2). These results provide critical new insights for the characterization and further development of efficient water-splitting photocatalysts from a dynamic perspective.
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