共查询到20条相似文献,搜索用时 15 毫秒
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Dr. Arik Kar Sumanta Sain Dr. Simanta Kundu Arka Bhattacharyya Dr. Swapan Kumar Pradhan Prof. Amitava Patra 《Chemphyschem》2015,16(5):1017-1025
Tuning the functional properties of nanocrystals is an important issue in nanoscience. Here, we are able to tune the photocatalytic properties of SnO2 nanocrystals by controlling their size and shape. A structural analysis was carried out by using X‐ray diffraction (XRD)/Rietveld and transmission electron microscopy (TEM). The results reveal that the number of oxygen‐related defects varies upon changing the size and shape of the nanocrystals, which eventually influences their photocatalytic properties. Time‐resolved spectroscopic studies of the carrier relaxation dynamics of the SnO2 nanocrystals further confirm that the electron–hole recombination process is controlled by oxygen/defect states, which can be tuned by changing the shape and size of the materials. The degradation of dyes (90 %) in the presence of SnO2 nanoparticles under UV light is comparable to that (88 %) in the presence of standard TiO2 Degussa P‐25 (P25) powders. The photocatalytic activity of the nanoparticles is significantly higher than those of nanorods and nanospheres because the effective charge separation in the SnO2 nanoparticles is controlled by defect states leading to enhanced photocatalytic properties. The size‐ and shape‐dependent photocatalytic properties of SnO2 nanocrystals make these materials interesting candidates for photocatalytic applications. 相似文献
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Electronic and Structural Properties of Highly Aluminum Ion Doped TiO2 Nanoparticles: A Combined Experimental and Theoretical Study 下载免费PDF全文
Desireé M. de los Santos Teresa Aguilar Dr. Antonio Sánchez‐Coronilla Dr. Javier Navas Dr. Norge Cruz Hernández Dr. Rodrigo Alcántara Dr. Concha Fernández‐Lorenzo Prof.Dr. Joaquín Martín‐Calleja 《Chemphyschem》2014,15(11):2267-2280
This study presents the experimental and theoretical study of highly internally Al‐doped TiO2 nanoparticles. Two synthesis methods were used and detailed characterization was performed. There were differences in the doping and the crystallinity, but the nanoparticles synthesized with the different methods share common features. Anatase to rutile transformation occurred at higher temperatures with Al doping. X‐ray photoelectron spectroscopy showed the generation of oxygen vacancies, which is an interesting feature in photocatalysis. In turn, the band‐gap energy and the valence band did not change appreciably. Periodic density functional calculations were performed to model the experimentally doped structures, the formation of the oxygen vacancies, and the band gap. Calculation of the density of states confirmed the experimental band‐gap energies. The theoretical results confirmed the presence of Ti4+ and Al3+. The charge density study and electron localization function analysis indicated that the inclusion of Al in the anatase structure resulted in a strengthening of the Ti?O bonds around the vacancy. 相似文献
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TiO2 doped with transition metals shows improved photocatalytic efficiency. Herein the electronic and optical properties of Mo‐doped TiO2 with defects are investigated by DFT calculations. For both rutile and anatase phases of TiO2, the bandgap decreases continuously with increasing Mo doping level. The 4d electrons of Mo introduce localized states into the forbidden band of TiO2, and this shifts the absorption edge into the visible‐light region and enhances the photocatalytic activity. Since defects are universally distributed in TiO2 or doped TiO2, the effect of oxygen deficiency due to oxygen vacancies or interstitial Mo atoms is systemically studied. Oxygen vacancies associated with the Mo dopant atoms or interstitial Mo will reduce the spin polarization and magnetic moment of Mo‐doped TiO2. Moreover, oxygen deficiency has a negative impact on the improved photocatalytic activity of Mo‐doped TiO2. The current results indicate that substitutional Mo, interstitial Mo, and oxygen vacancy have different impacts on the electronic/optical properties of TiO2 and are suited to different applications. 相似文献
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Jiaguo Yu Qin Li Shengwei Liu Mietek Jaroniec 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(7):2433-2441
Exploiting advanced photocatalysts under visible light is of primary significance for the development of environmentally relevant photocatalytic decontamination processes. In this study, the ionic liquid (IL), 1‐butyl‐3‐methylimidazolium tetrafluoroborate, was employed for the first time as both a structure‐directing agent and a dopant for the synthesis of novel fluorinated B/C‐codoped anatase TiO2 nanocrystals (TIL) through hydrothermal hydrolysis of tetrabutyl titanate. These TIL nanocrystals feature uniform crystallite and pore sizes and are stable with respect to phase transitions, crystal ripening, and pore collapse upon calcination treatment. More significantly, these nanocrystals possess abundant localized states and strong visible‐light absorption in a wide range of wavelengths. Because of synergic interactions between titania and codopants, the calcined TIL samples exhibited high visible‐light photocatalytic activity in the presence of oxidizing Rhodamine B (RhB). In particular, 300 °C‐calcined TIL was most photocatalytically active; its activity was much higher than that of TiO1.98N0.02 and reference samples (TW) obtained under identical conditions in the absence of ionic liquid. Furthermore, the possible photocatalytic oxidation mechanism and the active species involved in the RhB degradation photocatalyzed by the TIL samples were primarily investigated experimentally by using different scavengers. It was found that both holes and electrons, as well as their derived active species, such as .OH, contributed to the RhB degradation occurring on the fluorinated B/C‐codoped TiO2 photocatalyst, in terms of both the photocatalytic reaction dynamics and the reaction pathway. The synthesis of the aforementioned novel photocatalyst and the identification of specific active species involved in the photodegradation of dyes could shed new light on the design and synthesis of semiconductor materials with enhanced photocatalytic activity towards organic pollutants. 相似文献
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Enhanced Photoexcited Carrier Separation in Oxygen‐Doped ZnIn2S4 Nanosheets for Hydrogen Evolution 下载免费PDF全文
Wenlong Yang Lei Zhang Dr. Junfeng Xie Dr. Xiaodong Zhang Prof. Qinghua Liu Prof. Tao Yao Prof. Shiqiang Wei Prof. Qun Zhang Prof. Yi Xie 《Angewandte Chemie (International ed. in English)》2016,55(23):6716-6720
Limited by the relatively sluggish charge‐carrier separation in semiconductors, the photocatalytic performance is still far below what is expected. Herein, a model of ZnIn2S4 (ZIS) nanosheets with oxygen doping is put forward to obtain in‐depth understanding of the role that doping atoms play in photocatalysis. It shows enhanced photocatalytic activity compared with pristine ZIS. The electron dynamics analyzed by ultrafast transient absorption spectroscopy reveals that the average recovery lifetime of photoexcited electrons is increased by 1.53 times upon oxygen incorporation into the ZIS crystals, indicating enhanced separation of photoexcited carriers in oxygen‐doped ZIS nanosheets. As expected, the oxygen‐doped ZIS nanosheets show a remarkably improved photocatalytic activity with a hydrogen evolution rate of up to 2120 μmol h?1 g?1 under visible‐light irradiation, which is 4.5 times higher than that of the pristine ZIS nanosheets. 相似文献
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高度分散的Pt/TiO2的制备及光催化活性 总被引:7,自引:2,他引:7
用柠檬酸作为空穴捕获剂和分散剂,在温和条件下用光催化还原法将3nm金属铂沉积在7nm的锐钛矿相及介孔二氧化钛纳米晶表面,TEM观察显示铂的负载量为w=1.0%时,多数二氧化钛纳米晶表面沉积了岛状的铂团簇,XPS和电子衍射结果表明铂以游离态存在.负载w=1.0%~2.0%铂的TiO2在苯酚光氧化反应中活性显著提高,Pt/TiO2在氨气中经550℃氮化,可制得氮掺杂的Pt/TiO2可见光光催化剂,氮化过程中铂团簇没有烧结和显著长大。 相似文献
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Qin Xie Qiang‐Qiang Meng Gui‐Lin Zhuang Jian‐Guo Wang Xiao‐Nian Li 《International journal of quantum chemistry》2012,112(13):2585-2590
Photocatalytic splitting water into hydrogen and oxygen by utilizing solar energy is regarded as an effective strategy to solve oil crisis. By utilizing density functional calculations, we herein present the systemic studies with respect to water splitting mechanism on N‐doped TiO2 nanotube arrays (NTAs), and focus on activation energy, thermodynamic properties, and effects of N‐doping on reaction process. Our results reveal that the impurity 2p states of doped nitrogen effectively change electronic structure of TiO2 NTAs, which act as an electron acceptor and facilitate weakly bound electrons of valence band to be easily excited to acceptor level, as well as enhance the first H2O adsorption and dissociation on the inside wall of N‐doped TiO2 NTAs. Therefore, it is found that the rate‐determining step of water splitting is the formation reaction of HOO* on N‐doped TiO2 NTAs rather than the formation of HO* from the first H2O. © 2011 Wiley Periodicals, Inc. Int J Quantum Chem, 2011 相似文献
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Trapping of Oxygen Vacancies at Crystallographic Shear Planes in Acceptor‐Doped Pb‐Based Ferroelectrics 下载免费PDF全文
Dr. Dmitry Batuk Dr. Maria Batuk Dr. Alexander A. Tsirlin Prof. Dr. Joke Hadermann Dr. Artem M. Abakumov 《Angewandte Chemie (International ed. in English)》2015,54(49):14787-14790
The defect chemistry of the ferroelectric material PbTiO3 after doping with FeIII acceptor ions is reported. Using advanced transmission electron microscopy and powder X‐ray and neutron diffraction, we demonstrate that even at concentrations as low as circa 1.7 % (material composition approximately ABO2.95), the oxygen vacancies are trapped into extended planar defects, specifically crystallographic shear planes. We investigate the evolution of these defects upon doping and unravel their detailed atomic structure using the formalism of superspace crystallography, thus unveiling their role in nonstoichiometry in the Pb‐based perovskites. 相似文献
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Nana A. Kyeremateng Dr. Virginie Hornebecq Hervé Martinez Prof. Philippe Knauth Prof. Thierry Djenizian 《Chemphyschem》2012,13(16):3707-3713
Highly‐ordered Fe‐doped TiO2 nanotubes (TiO2nts) were fabricated by anodization of co‐sputtered Ti–Fe thin films in a glycerol electrolyte containing NH4F. The as‐sputtered Ti–Fe thin films correspond to a solid solution of Ti and Fe according to X‐ray diffraction. The Fe‐doped TiO2nts were studied in terms of composition, morphology and structure. The characterization included scanning electron microscopy, energy‐dispersive X‐ray spectroscopy, X‐ray diffraction, UV/Vis spectroscopy, X‐ray photoelectron spectroscopy and Mott–Schottky analysis. As a result of the Fe doping, an indirect bandgap of 3.0 eV was estimated using Tauc’s plot, and this substantial red‐shift extends its photoresponse to visible light. From the Mott–Schottky analysis, the flat‐band potential (Efb) and the charge carrier concentration (ND) were determined to be ?0.95 V vs Ag/AgCl and 5.0 ×1019 cm?3 respectively for the Fe‐doped TiO2nts, whilst for the undoped TiO2nts, Efb of ?0.85 V vs Ag/AgCl and ND of 6.5×1019 cm?3 were obtained. 相似文献
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Dr. Narayan Pradhan Samrat Das Adhikari Dr. Angshuman Nag Prof. D. D. Sarma 《Angewandte Chemie (International ed. in English)》2017,56(25):7038-7054
Introducing a few atoms of impurities or dopants in semiconductor nanocrystals can drastically alter the existing properties or even introduce new properties. For example, mid-gap states created by doping tremendously affect photocatalytic activities and surface controlled redox reactions, generate new emission centers, show thermometric optical switching, make FRET donors by enhancing the excited state lifetime, and also create localized surface plasmon resonance induced low energy absorption. In addition, researchers have more recently started focusing their attention on doped nanocrystals as an important and alternative material for solar energy conversion to meet the current demand for renewable energy. Moreover, the electrical and magnetic properties of the host are also strongly altered on doping. These beneficial dopant-induced changes suggest that doped nanocrystals with proper selections of dopant–host pairs may be helpful for generating designer materials for a wide range of current technological needs. How properties relate to the doping of a variety of semiconductor nanocrystals are summarized in this Review. 相似文献
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采用溶胶-凝胶法制备了Yb掺杂TiO2纳米光催化剂,并通过XRD和BET等手段进行了表征.以对苯二甲酸作为探针分子,结合化学荧光技术研究了光催化剂表面羟基自由基的生成;并以苯酚为光催化降解反应模型化合物,考察了光催化剂的活性.测定了苯酚在TiO2和Yb掺杂TiO2光催化剂上的吸附常数.结果表明:Yb掺杂使TiO2的粒径减小,比表面积增大,同时导致羟基自由基的生成速率增大.Yb掺杂有利于反应底物在催化剂表面的吸附,Yb的最佳掺入量为Yb/Ti摩尔比=0.8%. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(27):7900-7904
Visible‐light‐responsive reversible color‐switching systems are attractive to many applications because visible light has superior penetration and causes far less damage to organic molecules than UV. Herein, we report that self‐doping of SnO2−x nanocrystals with Sn2+ red‐shifts their absorption to the visible region and simultaneously produces oxygen vacancies, which can effectively scavenge photogenerated holes and thus enable the color switching of redox dyes using visible light. Wavelength‐selective switching can also be achieved by coupling the photocatalytic activity of the SnO2−x NCs with the color‐switching kinetics of different redox dyes. The fast light response enables the further fabrication of a solid film that can be repeatedly written on using a visible laser pen or projection printing through a photomask. This discovery represents a big step forward towards practical applications, especially in areas in which safety issues and photodamage by UV light are of concern. 相似文献
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波长对Ag/TiO2催化剂上二氧化碳光催化还原的影响 总被引:1,自引:0,他引:1
K.KOí K.ZATLOUKALOV L.OBALOV S.KREJíKOV Z.LACNY L.APEK A.HOSPODKOV O.OLCOV 《催化学报》2011,32(5):812-815
Photocatalytic reduction of CO2 by water was performed in the presence of a Ag/TiO2 catalyst under illumination by lamps with different wavelengths(254,365,and 400 nm).The yields of the main products(methane and methanol)were higher with the 254 nm lamp than with the 365 lamp while no products were observed with the 400 nm lamp.This was because the electron-hole generation rate increased with increasing energy of irradiation(decreasing wavelength)and there were higher densities of electron states at higher energies in TiO2. The increased efficiency of electron-hole generation with a shorter wavelength irradiation increased the efficiency of the catalyst.The energy of the electrons excited by visible light(400 nm)was too low for CO2 photocatalytic reduction. 相似文献
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Dr. Narayan Pradhan 《Chemphyschem》2016,17(8):1087-1094
Light‐emitting Mn‐doped semiconductor nanocrystals have been extensively studied for the last three decades for their intense and stable Mn d–d emission. In principle, this emission should be fixed at 585 nm (yellow), but recent studies have shown that the emission can be widely tuned even to 650 nm (red). This is a spectacular achievement as this would make Mn‐doped nanocrystals efficient and tunable light emitters. Keeping these developments in view, the chemistry of the synthesis of these materials, their photophysical processes and the expected origins of their red emission are summarized in this Minireview. All the related important studies from 1992 onwards are chronologically discussed, and one particular case is elaborated on in detail. As these materials are potentially important for biology, and photovoltaic, sensing and light‐emitting devices, this Minireview is expected to help researchers investigating the chemistry, physics and applications of these materials. 相似文献
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利用浸渍法制备了掺铜二氧化钛光催化剂,分别以乙酸降解和二氧化碳还原反应为探针,研究了催化剂的光催化氧化光催化还原性能.结果表明,铜掺杂能显著提高催化剂的光催化性能;结合光电子能谱、X光衍射分析等物理表征结果,对铜掺杂改性机制进行了讨论. 相似文献