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61.
Dr. Baoshun Liu Dr. Xuelei Wang Dr. Liping Wen Prof. Dr. Xiujian Zhao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(32):10751-10759
The in situ open‐circuit voltages (Voc) and the in situ photoconductivities have been measured to study electron behavior in photocatalysis and its effect on the photocatalytic oxidation of methanol. It was observed that electron injection to the conduction band (CB) of TiO2 under light illumination during photocatalysis includes two sources: from the valence band (VB) of TiO2 and from the methanol molecule. The electron injection from methanol to TiO2 is slower than that directly from the VB, which indicates that the adsorption mode of methanol on the TiO2 surface can change between dark and illuminated states. The electron injection from methanol to the CB of TiO2 leads to the upshift of the Fermi level of electrons in TiO2, which is the thermodynamic driving force of photocatalytic oxidation. It was also found that the charge state of nano‐TiO2 is continuously changing during photocatalysis as electrons are injected from methanol to TiO2. Combined with the apparent Langmuir–Hinshelwood kinetic model, the relation between photocatalytic kinetics and electrons in the TiO2 CB was developed and verified experimentally. The photocatalytic rate constant is the variation of the Fermi level with time, based on which a new method was developed to calculate the photocatalytic kinetic rate constant by monitoring the change of Voc with time during photocatalysis. 相似文献
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Hui Qiang Tao Chen Zhuo Wang Wenqian Li Yunzhe Guo Jie Yang Xueshun Jia Hui Yang Weibo Hu Ke Wen 《中国化学快报》2021,31(12):3225-3229
The development of heterogeneous catalysts with substrate shape, size or electronic constitution selectivity is a huge challenge in photocatalysis. Reported herein is a host-guest interaction strategy to endow photocatalysts with special selectivity. By adjusting the precursors, conjugated macrocycle polymers (CMPs) with pillar[5]arene struts (CMP-1 and CMP-2) and a corresponding non-pillar[5]arene-contained conjugated organic polymer (COP-1) were prepared and the photocatalytic activities toward sulfide derivatives were investigated. The sulfides showed similar conversions when COP-1 was used as a photocatalyst, but exhibited significant differences when it turned to the CMPs. Remarkably, the conversion yield of S-1 achieved near 18 folds over the one of S-2 when CMP-2 was used as a catalyst. Mechanism studies confirmed that the “host-guest” effect of pillar[5]arene struts in CMPs was the main cause of the difference. The present work establishes CMPs as novel heterogeneous photocatalysts with substrate selectivity, and such a method will inspire the researchers concerning preparation of heterogeneous catalysts with excellent selectivity. 相似文献
65.
制备了四碘化5,10,15,20-四(对-N,N,N三甲基苯胺基)卟啉敏化的钛酸盐纳米管(TAPPI-TNTs),并利用甲基橙(MO)作为模型污染物考察了其可见光催化活性。结果表明,TAPPI-TNTs是一个高效的可见光催化剂,在其催化作用下,可见光照射1 h后,甲基橙的降解率为89%。与此相反,纯钛酸盐纳米管并不具有可见光催化活性。此外,TAPPI-TNTs的稳定性较高,可以多次循环使用,在第五次循环中,甲基橙的降解率仍可达到50%以上。这可能是由于带正电荷的卟啉与带负电荷的钛酸盐纳米管之间存在着较强的静电吸引作用,卟啉紧密地吸附在钛酸盐纳米管上,导致卟啉的光激发电子易于向钛酸盐纳米管转移,从而使钛酸盐纳米管得到了有效敏化。 相似文献
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V. V. Shvalagin A. L. Stroyuk S. Ya. Kuchmii 《Theoretical and Experimental Chemistry》2004,40(6):378-382
Cathodic photocorrosion occurs upon stationary photoirradiation of ethanolic ZnO sols. The photocorrosion rate increases with decreasing particle size. This effect due to the appearance of quantum-sized effects in ZnO nanocrystals results from an increase in the reduction potential of the semiconductor upon irradiation, which may exceed the Fermi level for cathodic decomposition of zinc oxide nanoparticles.Translated from Teoreticheskaya i Éksperimentalnaya Khimiya, Vol.40, No.6, pp. 363–367, November–December, 2004. 相似文献
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Sajjad S Leghari SA Chen F Zhang J 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(46):13795-13804
A controllable and reproducible synthesis of highly ordered two-dimensional hexagonal mesoporous, crystalline bismuth-doped TiO(2) nanocomposites with variable Bi ratios is reported here. Analyses by transmission electron microscopy, X-ray diffraction, Raman, and X-ray photoelectron spectroscopy reveal that the well-ordered mesostructure is doped with Bi, which exists as Bi(3+) and Bi((3+x+)). The Bi-doped mesoporous TiO(2) (ms-TiO(2)) samples exhibit improved photocatalytic activities for simultaneous phenol oxidation and chromium reduction in aqueous suspension under visible and UV light over the pure ms-TiO(2), P-25, and conventional Bi-doped titania. The high catalytic activity is due to both the unique structural characteristics and the Bi doping. This new material extends the spectral response from UV to the visible region, and reduces electron-hole recombination, which renders the 2.0% Bi-doped ms-TiO(2) photocatalyst highly responsive to visible light. 相似文献
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Arun Kumar Sinha Mrinmoyee Basu Mukul Pradhan Sougata Sarkar Tarasankar Pal Prof. 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(26):7865-7874
We report here the preparation of a crystalline, pure hexagonal phase of ZnO as hollow 500–800 nm spheroids in the presence of organic bases, such as pyridine, using zinc acetate as the precursor salt. The spheroids exhibit unique 3D hierarchical architectures, like cocoons, and demonstrate improved superhydrophobic (water contact angle, 150°) character due to the inherited air‐trapped capillarity within the cocoon structure. The simple synthetic strategy used in this process is modified hydrothermolysis (MHT), which represents a general approach and may contribute to the formation mechanism of the hollow nanostructures with highly improved porosity. Depending on the concentration of the precursor salt, it has been possible to cover glass plates or the inner wall of a reaction vessel with ZnO nanocrystals. A low salt concentration (<0.01 M ) allows the easy preparation of a superhydrophobic glass surface, whereas a high salt concentration (>0.01 M ) results in the precipitation of cocoons at the bottom of the reaction vessel as a solid mass together with a deposited thin film of ZnO nanocrystals covering the inner wall of the glass vessel. The thickness of the film successively grows through repetitive hydrothermolysis processes for which a low salt concentration (<0.01 M ) was employed. Because of the hollow cocoonlike morphology, the surface area of the film is greatly increased, which makes it accessible for functionalization by incoming substrates from both sides (internally and externally) and helps to drive a competent photocatalytic dye degradation pathway. The heterocyclic base pyridine exclusively develops cocoons. Thus, the mechanism of self‐aggregation of ZnO nanocrystals under MHT reaction conditions has been studied and the characterization of the compounds has been supported with physical measurements. 相似文献
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