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

Huang, Jiaquan; Zhao, Xinyi; Huang, Xunkun; Liang, WanZhen

doi:10.1039/d1cp03509f

Cited by 11 publications

(11 citation statements)

References 62 publications

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“…These applications of ML in modeling atomic FFs are successful in predicting the structural dynamics and total energy of molecules and bulk systems. − A description of excited electronic states with ML is more challenging because they are more complex functions of system geometries than ground states. Particularly relevant for solar energy applications are ML efforts to extend the range of nonadiabatic MD simulations, which allow one to model charge separation, trapping, and recombination processes that govern solar cell efficiencies. − ,− …”

mentioning

confidence: 99%

Electron-Volt Fluctuation of Defect Levels in Metal Halide Perovskites on a 100 ps Time Scale

Wang

Chu

et al. 2022

J. Phys. Chem. Lett.

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Metal halide perovskites (MHPs) have gained considerable attention due to their excellent optoelectronic performance, which is often attributed to unusual defect properties. We demonstrate that midgap defect levels can exhibit very large and slow energy fluctuations associated with anharmonic acoustic motions. Therefore, care should be taken classifying MHP defects as deep or shallow, since shallow defects may become deep and vice versa. As a consequence, charges from deep levels can escape into bands, and light absorption can be extended to longer wavelengths, improving material performance. The phenomenon, demonstrated with iodine vacancy in CH 3 NH 3 PbI 3 using a machine learning force field, can be expected for a variety of defects and dopants in many MHPs and other soft inorganic semiconductors. Since large-scale anharmonic motions can be precursors to chemical decomposition, a known problem with MHPs, we propose that materials that are stiffer than MHPs but softer than traditional inorganic semiconductors, such as Si and TiO 2 , may simultaneously exhibit excellent performance and stability.

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confidence: 99%

Electron-Volt Fluctuation of Defect Levels in Metal Halide Perovskites on a 100 ps Time Scale

Wang

Chu

et al. 2022

J. Phys. Chem. Lett.

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“…Conversely, for CO 2 reduction, a photocatalyst with high CO affinity led to high reaction yields and selectivity toward reduction to CH 4 . 18,67−69 Our evidence suggests that CO 53,56,74 However, these studies focus on the charge transfer mechanism. Our approach represents a complementary mechanism where the O−H symmetric bond stretching activation could play a role in plasmon enhanced water splitting.…”

mentioning

confidence: 90%

“…The predominant activation of such a mode is coherent with calculations on a charged water molecule (see the Supporting Information). The fact that HCs can effectively activate water splitting reactions is well established − and a few computational studies were conducted to study the HC–water interaction. ,, However, these studies focus on the charge transfer mechanism. Our approach represents a complementary mechanism where the O–H symmetric bond stretching activation could play a role in plasmon enhanced water splitting.…”

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confidence: 99%

Energy Transfer to Molecular Adsorbates by Transient Hot Electron Spillover

et al. 2023

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Hot electron (HE) photocatalysis is one of the most intriguing fields of nanoscience, with a clear potential for technological impact. Despite much effort, the mechanisms of HE photocatalysis are not fully understood. Here we investigate a mechanism based on transient electron spillover on a molecule and subsequent energy release into vibrational modes. We use state-of-the-art real-time Time Dependent Density Functional Theory (rt-TDDFT), simulating the dynamics of a HE moving within linear chains of Ag or Au atoms, on which CO, N 2 , or H 2 O are adsorbed. We estimate the energy a HE can release into adsorbate vibrational modes and show that certain modes are selectively activated. The energy transfer strongly depends on the adsorbate, the metal, and the HE energy. Considering a cumulative effect from multiple HEs, we estimate this mechanism can transfer tenths of an eV to molecular vibrations and could play an important role in HE photocatalysis.

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“…The advantages of the direct electron transfer method offer high transfer productivity with less energy loss. The significant energy loss in indirect transfer arises from the injection of hot electrons across the heterojunction surface, and from the scattering of electrons and phonons in the electronic state before the transfer [ 56 , 57 ]. During the direct injection process, Landau damping is used to generate hot electrons in the hybridized orbitals directly on the direct electron transfer path to prevent energy loss [ 58 ].…”

Section: Plasmonic Effect For Photocatalytic Degradationmentioning

confidence: 99%

A review on plasmonic-based heterojunction photocatalysts for degradation of organic pollutants in wastewater

et al. 2023

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Organic pollutants in wastewater are the biggest problem facing the world today due to population growth, rapid increase in industrialization, urbanization, and technological advancement. There have been numerous attempts to use conventional wastewater treatment techniques to address the issue of worldwide water contamination. However, conventional wastewater treatment has a number of shortcomings, including high operating costs, low efficiency, difficult preparation, fast recombination of charge carriers, generation of secondary waste, and limited light absorption. Therefore, plasmonic-based heterojunction photocatalysts have attracted much attention as a promising method to reduce organic pollutant problems in water due to their excellent efficiency, low operating cost, ease of fabrication, and environmental friendliness. In addition, plasmonic-based heterojunction photocatalysts contain a local surface plasmon resonance that enhances the performance of photocatalysts by improving light absorption and separation of photoexcited charge carriers. This review summarizes the major plasmonic effects in photocatalysts, including hot electron, local field effect, and photothermal effect, and explains the plasmonic-based heterojunction photocatalysts with five junction systems for the degradation of pollutants. Recent work on the development of plasmonic-based heterojunction photocatalysts for the degradation of various organic pollutants in wastewater is also discussed. Lastly, the conclusions and challenges are briefly described and the direction of future development of heterojunction photocatalysts with plasmonic materials is explored. This review could serve as a guide for the understanding, investigation, and construction of plasmonic-based heterojunction photocatalysts for various organic pollutants degradation. Graphical abstract Herein, the plasmonic effects in photocatalysts, such as hot electrons, local field effect, and photothermal effect, as well as the plasmonic-based heterojunction photocatalysts with five junction systems for the degradation of pollutants are explained. Recent work on plasmonic-based heterojunction photocatalysts for the degradation of various organic pollutants in wastewater such as dyes, pesticides, phenols, and antibiotics is discussed. Challenges and future developments are also described.

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

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...

Cited by 11 publications

References 62 publications

Electron-Volt Fluctuation of Defect Levels in Metal Halide Perovskites on a 100 ps Time Scale

Electron-Volt Fluctuation of Defect Levels in Metal Halide Perovskites on a 100 ps Time Scale

Energy Transfer to Molecular Adsorbates by Transient Hot Electron Spillover

A review on plasmonic-based heterojunction photocatalysts for degradation of organic pollutants in wastewater

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