Relating surface defect energetics with reactant gas adsorption during the photo-catalytic reduction of CO2 by partially hydrolyzed In2O3 nanorods

文献信息

发布日期 2020-08-28

DOI 10.1039/D0CP03217D

影响因子 3.676

作者

Joel Y. Y. Loh

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摘要

Photo-Induced Transient Current Spectroscopy (PICTS) is a versatile technique for measurements of defect state energies and densities in photo-active materials. It is suitable for investigating the surface-gas adsorbate behavior and the defect characteristics of defect laden In2O3−x(OH)y nanorods, having oxygen vacancies and hydroxide surface groups, under in situ reactor conditions of dark ambient temperature, dark 150 °C and photo-illuminated 150 °C, for the photo-assisted Reverse Water Gas Shift reaction. From glovebox-protected X-ray Photoelectron Spectroscopy and in situ PICTS measurements we determined that the reduction of CO2 is associated with heterolytic dissociation of H2 into In–H§− and HO–H§+ centres accompanied by an increase in average carrier trap energies; increased carbonate formation in a photo/thermal reactor state of H2 + CO2, and an average trap energy decrease of 0.11 eV from H2 to a CO2 + H2 mixture, which correlates with binding energy shifts of the OH shoulder of the O1s spectra. These results show the reactivity link between the various OH groups, oxygen vacancies and trap energies of In2O3−x(OH)y in the reactant gas atmosphere components.

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来源期刊

Physical Chemistry Chemical Physics

CiteScore: 5.5

自引率: 10.3%

年发文量: 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.