Oxygen vacancies as active sites for H2S dissociation on the rutile TiO2(110) surface: a first-principles study
文献信息
Shiqian Wei, Zhi Zhang, Great R. Patzke
Spin-polarized DFT+U computations have been performed to investigate the role of oxygen vacancies in dissociating H2S on the rutile TiO2(110) surface. A bridged O2c atom is demonstrated to be the most energetically favorable oxygen vacancy site, which makes V(O2c) an electron donator center and induces an isolated defect level with narrowed band gaps. A H2S molecule is adsorbed dissociatively over V(O2c), but molecularly on the perfect surface. For H2S dissociation, the HS/H intermediate state reveals the best thermal stability on both defected and perfect surfaces. Moreover, potential energy surface analysis shows that V(O2c) reduces markedly the energy barriers for the paths along H2S dissociation. This indicates oxygen vacancies to be efficient trap centers for H2S dissociation, as evidenced by a significant interfacial charge transfer promoted by vacancies. This work could provide insights into the role of oxygen vacancies in facilitating the decomposition of H2S on rutile TiO2(110) surface.
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Physical Chemistry Chemical Physics

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.













