SiO2 coated pure and doped titania pigments: low temperature CVD deposition and quantum chemical study

文献信息

发布日期 2011-10-24
DOI 10.1039/C1CP22681A
影响因子 3.676
作者

Darren J. Simpson, Alagu Thilagam, Giuseppe P. Cavallaro, Klara Kaplun, Andrea R. Gerson


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摘要

We report the in-flight CVD coating with smooth 1–2 nm thick SiO2 of pure and doped rutile particles via the oxidation of SiCl4 vapour introduced in the high temperature zone of a purpose built thermal reactor. The effectiveness of the coatings was determined by a combination of electron microscopy, surface analysis and photocatalytic measurements. No excess Cl was detected on the coated pigment particles indicating the complete oxidation of the SiCl4 precursor. In conjunction with the experimental outcomes of this optimised deposition process, we use first-principles density functional and semi-empirical quantum chemical calculations to examine the underlying electronic processes which determined the morphology and photocatalytic properties of the coated titania. We highlight the presence of low lying valence electronic states which reduce photocatalytic activity, and as a consequence decrease the population of photo-excited titania electrons which transfer to the surrounding matrix. Born–Oppenheimer molecular dynamics (MD) simulations indicate that the coating process is completed within the order of 10 ps.

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来源期刊

Physical Chemistry Chemical Physics

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.

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