Journal ArticleDOI
Role of oxygen vacancies in photocatalytic water oxidation on ceria oxide: Experiment and DFT studies
TLDR
In this paper, the critical role of oxygen vacancies in photocatalytic water oxidation was investigated using a one-step hydrothermal method with in-situ reducing treatment.Abstract:
Photocatalytic water oxidation suffers from sluggish kinetics and remains the bottleneck for water splitting. Here, using CeO 2 nanorods as model photocatalyst we studied the critical role of oxygen vacancies in photocatalytic water oxidation. First CeO 2 nanorods with similar morphology but different concentration of oxygen vacancies were fabricated by one-step hydrothermal method with in-situ reducing treatment. The optical absorption, charge transfer efficiency, and photocatalytic activity in oxygen generation were found closely dependent on the concentration of oxygen vacancies. Then density functional theory calculations were conducted to unveil the role of oxygen vacancies and understand the water oxidation mechanism. It was found the presence of oxygen vacancies narrows the bandgap and modulates the electronic structure for accelerating the charge transfer, in good agreement with the experimental observations. The overall oxygen generation pathway was screened and the oxygen vacancies were found to lower the barrier energy for the rate limiting step of O O bond formation and restrain the reverse reaction of O and H, thus the O 2 generation kinetics on oxygen-defective CeO 2 are improved significantly. This study provides in-depth understanding on the critical role of oxygen vacancies in photocatalytic water oxidation and is helpful for designing highly efficient photocatalyst to overcome the bottleneck of water splitting.read more
Citations
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Journal ArticleDOI
Defect engineering in photocatalytic materials
TL;DR: In this paper, the state-of-the-art progress on defect-engineered photocatalytic materials is reviewed and the future opportunities and challenges regarding defect engineering in photocatalysis are highlighted.
Journal ArticleDOI
Highly efficient mesoporous MnO2 catalysts for the total toluene oxidation: Oxygen-Vacancy defect engineering and involved intermediates using in situ DRIFTS
Shengpeng Mo,Qi Zhang,Jiaqi Li,Yuhai Sun,Quanming Ren,Sibei Zou,Qian Zhang,Jiahui Lu,Mingli Fu,Deqing Mo,Junliang Wu,Haomin Huang,Daiqi Ye +12 more
TL;DR: In this paper, the role of oxygen vacancy defects in the activation-oxidation process of toluene was investigated, and the as-prepared MnOx-ET catalyst has more surficial oxygen vacancies and good oxygen storage capacity.
Journal ArticleDOI
Synthesis of Bi2WO6 with gradient oxygen vacancies for highly photocatalytic NO oxidation and mechanism study
TL;DR: In this paper, the formation of oxygen vacancy defects in BWO is responsible for the tuning band structure and modifying surface chemical state to improve carriers separation efficiency, enlarge visible light absorption range and facilitate reactant activation.
Journal ArticleDOI
3D hierarchical H2-reduced Mn-doped CeO2 microflowers assembled from nanotubes as a high-performance Fenton-like photocatalyst for tetracycline antibiotics degradation
Anqi Wang,Zhikeng Zheng,Hui Wang,Yuwen Chen,Chenghui Luo,Dingjun Liang,Bowen Hu,Rongliang Qiu,Kai Yan +8 more
TL;DR: In this article, a Fenton-photocatalysis synergy holds great promising for environment remediation, and offer a feasible means to tune the performance of CeO2-based materials especially in Fentonlike photocatalytic oxidation of antibiotics.
Journal ArticleDOI
Structure-Activity Relationship of Defective Metal-Based Photocatalysts for Water Splitting: Experimental and Theoretical Perspectives.
TL;DR: This work comprehensively reviews point defective metal‐based photocatalysts for water splitting, focusing on understanding the defects' disorder effect on optical adsorption, charge separation and migration, and surface reaction.
References
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Journal ArticleDOI
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set.
Georg Kresse,Jürgen Furthmüller +1 more
TL;DR: An efficient scheme for calculating the Kohn-Sham ground state of metallic systems using pseudopotentials and a plane-wave basis set is presented and the application of Pulay's DIIS method to the iterative diagonalization of large matrices will be discussed.
Journal ArticleDOI
Accurate and simple analytic representation of the electron-gas correlation energy
John P. Perdew,Yue Wang +1 more
TL;DR: A simple analytic representation of the correlation energy for a uniform electron gas, as a function of density parameter and relative spin polarization \ensuremath{\zeta}, which confirms the practical accuracy of the VWN and PZ representations and eliminates some minor problems.
Journal ArticleDOI
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
Sergei L. Dudarev,Gianluigi A. Botton,Sergey Y. Savrasov,Colin J. Humphreys,Adrian P. Sutton +4 more
TL;DR: In this article, the authors improved the description of both electron energy loss spectra and parameters characterizing the structural stability of the material compared with local spin density functional theory by taking better account of electron correlations in the $3d$ shell of metal ions in nickel oxide.
Journal ArticleDOI
A fast and robust algorithm for Bader decomposition of charge density
TL;DR: In this article, an algorithm for decomposition of electronic charge density into atomic contributions is presented. But instead of explicitly finding and representing the dividing surfaces, which is a challenging task, the algorithm assigns each point on a regular (x,y,z) grid to one of the regions by following a steepest ascent path on the grid.
Journal ArticleDOI
Ab initio molecular dynamics for open-shell transition metals.
Georg Kresse,Jürgen Hafner +1 more
TL;DR: In this paper, it was shown that quantum-mechanical molecular-dynamics simulations in a finite-temperature local density approximation based on the calculation of the electronic ground state and of the Hellmann-Feynman forces after each time step are feasible for liquid noble and transition metals.
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