Understanding the mechanism of plasmon-driven water splitting: hot electron injection and a near field enhancement effect

Literature Information

Publication Date 2021-10-26
DOI 10.1039/D1CP03509F
Impact Factor 3.676
Authors

Jiaquan Huang, Xinyi Zhao, Xunkun Huang, WanZhen Liang


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Abstract

Utilizing plasmon-generated hot carriers to drive chemical reactions has currently become an active area of research in solar photocatalysis at the nanoscale. However, the mechanism underlying exact transfer and the generation dynamics of hot carriers, and the strategies used to further improve the quantum efficiency of the photocatalytic reaction still deserve further investigation. In this work, we perform a nonadiabatic excited-state dynamics study to depict the correlation between the reaction rate of plasmon-driven water splitting (PDWS) and the sizes of gold particles, the incident light frequency and intensity, and the near-field spatial distribution. Four model systems, H2O and Au20@H2O separately interacting with the laser field and the near field generated by the Au nanoparticle (NP) with a few nanometers in size, have been investigated. Our simulated results clearly unveil the mechanism of PDWS and hot-electron injection in a Schottky-free junction: the electrons populated on the antibonding orbitals of H2O are mandatory to drive the OH bond breaking and the strong orbital hybridization between Au20 and H2O creates the conditions for direct electron injection. We further find that the linear dependence of the reaction rate and the field amplitude only holds at a relatively weak field and it breaks down when the second OH bond begins to dissociate and field-induced water fragmentation occurs at a very intensive field, and that with the guarantee of electron injection, the water splitting rate increases with an increase in the NP size. This study will be helpful for further improving the efficiency of photochemical reactions involving plasmon-generated hot carriers and expanding the applications of hot carriers in a variety of chemical reactions.

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Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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