Direct splitting of water under visible light irradiation with an oxide semiconductor photocatalyst.

The photocatalytic splitting of water into hydrogen and oxygen using solar energy is a potentially clean and renewable source for hydrogen fuel. The first photocatalysts suitable for water splitting, or for activating hydrogen production from carbohydrate compounds made by plants from water and carbon dioxide, were developed several decades ago. But these catalysts operate with ultraviolet light, which accounts for only 4% of the incoming solar energy and thus renders the overall process impractical. For this reason, considerable efforts have been invested in developing photocatalysts capable of using the less energetic but more abundant visible light, which accounts for about 43% of the incoming solar energy. However, systems that are sufficiently stable and efficient for practical use have not yet been realized. Here we show that doping of indium-tantalum-oxide with nickel yields a series of photocatalysts, In(1-x)Ni(x)TaO(4) (x = 0-0.2), which induces direct splitting of water into stoichiometric amounts of oxygen and hydrogen under visible light irradiation with a quantum yield of about 0.66%. Our findings suggest that the use of solar energy for photocatalytic water splitting might provide a viable source for 'clean' hydrogen fuel, once the catalytic efficiency of the semiconductor system has been improved by increasing its surface area and suitable modifications of the surface sites.     

新型可见光激发解水材料的研究进展

直接利用太阳光激发光催化剂分解水得到氢气和氧气,是极具诱惑力的一个研究方向,而目前面临的难点之一是已发现的光催化剂难以在可见光激发下具有持续、稳定的性能和较高的分解水的效率,因此找到新的可见光激发光催化剂是非常必要的.本文介绍了该领域的最新研究成果,并对可见光光激发催化剂分解水的机理进行了阐述.     

Sn/Sn_3O_(4-x) heterostructure rich in oxygen vacancies with enhanced visible light photocatalytic oxidation performance

Sn_3O_4, a common two-dimensional semiconductor photocatalyst, can absorb visible light.However, owing to its rapid recombination of photogenerated electron-hole pairs, its absorption is not sufficient for practical application.In this work, a Sn nanoparticle/Sn_3O_(4-x) nanosheet heterostructure was prepared by in situ reduction of Sn_3O_4 under a H_2 atmosphere.The Schottky junctions formed between Sn and Sn_3O_(4-x) can enhance the photogenerated carrier separation ability.During the hydrogenation process, a portion of the oxygen in the semiconductor can be extracted by hydrogen to form water, resulting in an increase in oxygen vacancies in the semiconductor.The heterostructure showed the ability to remove Rhodamine B.Cell cytocompatibility experiments proved that Sn/Sn_3O_(4-x) can significantly enhance cell compatibility and reduce harm to organisms.This work provides a new method for the fabrication of a Schottky junction composite photocatalyst rich in oxygen vacancies with enhanced photocatalytic performance.     

Cu,In-ZnSeS催化剂的制备及其光解水制氢性能的研究

采用化学共沉淀法制备了掺杂CuI、n的ZnSeS半导体光催化剂,并通过X射线粉末衍射、紫外-可见漫反射光谱和比表面积与孔径分析、X射线荧光光谱、热质量损失(热失重)分析对催化剂的结构进行了表征.在自制的反应装置上评价了催化剂的光分解水产氢性能.结果表明:在Cu,In-ZnSeS中掺杂CuI、n的摩尔分数为2%时其光吸收性能最好,最大吸收边红移至700 nm;紫外光照射下该催化剂光分解水产氢的量子效率达到4.83%;催化剂具有良好的热稳定性和光学稳定性,反应100 h其产氢性能没有衰减.     

新型AgBr/GO复合催化剂的制备及其可见光催化还原CO2性能的初步研究

 采用液相合成法,在十三烷基三甲基溴化铵（CTAB）辅助下制备具有可见光效应的AgBr/GO复合材料,并考察其在可见光下催化还原CO₂制备碳氢化合物的可行性及催化性能。XRD和TEM结果表明：AgBr纳米颗粒均匀地分散在GO载体表面,有利于光诱导下产生的电荷在AgBr与GO界面间的有效传递。可见光照射下,AgBr/GO复合催化剂还原CO₂生成的甲烷、甲醇、CO和乙醇的产量分别是106.11、64.20、26.53和10.96 μmol·g^-1,明显高于AgBr的催化活性。AgBr/GO在重复使用5次后其光催化还原CO₂的活性基本保持不变,因此AgBr/GO是一种高效的、光化学性质稳定的催化剂。     

掺杂铕氧化铋光催化剂的制备及其可见光的光催化性能

通过在Bi2O3中掺杂稀土元素Eu, 以甲基橙为目标污染物, 考察稀土掺杂比、 离子液体浓度、 灼烧温度、 灼烧时间和催化剂投加量对光催化效
果的影响, 并利用X射线衍射(XRD)和紫外 可见漫反射光谱(UV-Vis DRS)研究样品结构. 结果表明: 最佳制备条件为n(Eu)∶n(Bi)=0.25, 离子液体浓度为0.002 5 mol/L, 灼烧温度为400 ℃, 灼烧时间为5 h, 最佳投加量为5.0 g/L; 在最佳制备条件下制得的光催化剂在可见光光源下对甲基橙的降解率为92.57%, 远高于未掺杂Eu光催化剂的降解率(29.26%); 制备的催化剂为四方晶系, 吸收边带红移约120 nm, 禁带宽度由2.86 eV变为2.37 eV. 即掺杂Eu可扩展光的响应范围, 提高Bi₂O₃的光催化活性.     

Sn/Sn3O4?x heterostructure rich in oxygen vacancies with enhanced visible light photocatalytic oxidation performance

Sn3O4,a common two-dimensional semiconductor photocatalyst,can absorb visible light.However,owing to its rapid recombina-tion of photogenerated electron?hole pairs,its absorption is not sufficient for practical application.In this work,a Sn nanoparticle/Sn3O4?x nanosheetheterostructurewaspreparedbyin situreductionofSn3O4underaH2atmosphere.TheSchottkyjunctionsformedbetweenSnand Sn3O4?x can enhance the photogenerated carrier separation ability.During the hydrogenation process,a portion of the oxygen in the semicon-ductor can be extracted by hydrogen to form water,resulting in an increase in oxygen vacancies in the semiconductor.The heterostructure showed the ability to remove Rhodamine B.Cell cytocompatibility experiments proved that Sn/Sn3O4?x can significantly enhance cell compat-ibility and reduce harm to organisms.This work provides a new method for the fabrication of a Schottky junction composite photocatalyst rich in oxygen vacancies with enhanced photocatalytic performance.     

光催化剂可见光化研究进展

 光催化剂可将光能转变为化学能,可用于使水分解制氢及将环境中的有害物还原氧化为无害物质等,其应用前景十分广阔.而阻碍其应用的是不能有效地利用太阳光,因此研究开发可见光化的光催化剂就成为当前光催化剂研究中最重要的课题.本文简述了光催化剂的作用原理及较系统地介绍了可见光化光催化剂目前的研究现状及成果.     

氮化碳光催化分解水研究进展

光能取之不尽用之不竭,利用光催化技术分解水解制氢被认为是解决能源与环境问题的有效手段之一。2009年,氮化碳聚合物半导体实现了光催化产氧与产氢水分解半反应,打破了人们对有机聚合物半导体不宜作为光催化材料的传统认识。氮化碳材料由碳、氮两种元素构成,廉价易得,且光化学性质稳定。近年来,以氮化碳为代表的不含金属组分的光催化材料逐渐成为国际光催化研究的热点之一。本文将从氮化碳材料的光催化分解水的构-效关系出发,围绕共聚合氮化碳、结晶相氮化碳和氮化碳光电极,讨论氮化碳材料在光催化分解水的研究现状与发展趋势。     

Magnetically separable and visible light-active Ag/NiCo_2O_4 nanorods prepared by a simple route for superior photodegradation of atrazine in water

Atrazine(ATZ) is a known herbicide used in agriculture and caused many concerns according to its toxicity.Herein,we have prepared NiCo_2 O_4 nanorods that can work as a photocatalyst under visible light exposure by Ag loading through a simple route.The characterizations revealed the role of Ag for improving the structural,optical and optoelectronic properties of the produced photocatalyst.The Ag loading with 5 wt% confirms the minimization of the bandgap from 3.6 down to 2.57 eV with enhanced visible light absorption and sustaining the magnetic properties.The Ag/NiCo_2 O_4 nanorods showed a superior photodegradation of ATZ within 20 min at2.0 g L~(-1) with excellent recyclability.The enhancement of the photocatalytic activity is referred to the local surface plasmon resonance of Ag-loaded photocatalyst.This reduces the electron-hole recombination and outperforms the unloaded sample.This work is highlighting the application of magnetically separable spinel photocatalysts for the removal of herbicides and water remediation.     

LaCo1-xCuxO3纳米晶对染料酸性黑10B的光催化降解研究

采用EDTA络合溶胶-凝胶法在较低的温度下合成了LaCo1-xCuxO3复合氧化物纳米晶,通过XRD和SEM等手段对LaCo1-xCuxO3进行了表征.结果表明:在600℃焙烧即可得到钙钛矿型LaCo1-xCuxO3纳米晶,700℃焙烧所得颗粒基本呈球形,粒径为50 nm左右.采用IR和UV-Vis技术研究了该系列纳米晶对染料酸性黑10B的光催化降解活性,结果表明:掺杂量、焙烧温度、催化剂用量、光照时间等因素对脱色率均有一定的影响,在适宜的实验条件下,可使酸性黑10B的脱色率接近100%.     

固相法制备新型KNN基近红外透明陶瓷

采用传统固相烧结工艺,注重烧结时的气氛控制,制备了铌酸钾钠(KNN)基无铅透明陶瓷xBa(Sc0.5Nb0.5)O3-(1-x)(K0.5N0.5)NbO3.并对其相结钩、微观结构、压电性能和透光率进行了研究.结果表明:该体系陶瓷具有准立方钙钛矿结构,没有其他杂相,晶粒大小与可见光波长相当,高度致密,无明显的晶界存在.在x=0.05时,d33最高可达到110 pC/N.同时该材料具有良好的透明性,在可见光范围内,透过率达到47％左右,近红外2500 nm处,透过率接近70％,是一种有望取代铅基透明陶瓷的环境友好型无铅透明陶瓷.     

碘掺杂Bi4O5Br2可见光催化降解2,4-二羟基苯甲酸甲酯

2,4-二羟基苯甲酸甲酯（MDB）,是对羟基苯甲酸甲酯在高级氧化过程中形成的的较稳定中间产物,具有比甲酯更强的毒性,其在环境中的存在对水资源及生态系统具有较高的潜在风险. 本文首次在可见光照射下催化降解2,4-二羟基苯甲酸甲酯,并取得了较好的进展. 与纯Bi4O5Br2相比,I-doped Bi4O5Br2催化剂表现出优异的可见光降解2,4-二羟基苯甲酸甲酯活性,其降解速率接近是纯Bi4O5Br2的5倍（0.038 min-1）. I-doped Bi4O5Br2光催化活性增强的主要原因是其更佳的光生电子空穴对的分离效率和更宽的光吸收范围. 机理研究表明,光生空穴和超氧自由基为MDB可见光催化降解过程中的主要活性氧化物种.     

三维g-C3N4/NixP复合光催化剂的制备及其可见光下产氢性能的研究

以三聚氰胺和三聚氰酸为原料,以水为溶剂采用超分子自组装法制备三维互联框架形貌的3D g-C₃N₄（DCN）。以次磷酸钠和硫酸镍作为磷源和镍源,采用原位光沉积法在3D g-C₃N₄上沉积Ni_xP,制备了3D g-C₃N₄/Ni_xP复合光催化剂。采用扫描电子显微镜（SEM）、透射电子显微镜（TEM）、X射线衍射（XRD）、傅里叶变换红外光谱（FT-IR）、X射线光电子能谱（XPS）、紫外可见漫反射光谱（UV-Vis DRS）等手段对样品进行了表征,结果表明,3D g-C₃N₄/Ni_xP复合光催化剂上均匀负载着直径几十纳米的Ni_xP颗粒并且Ni_xP表现为无定形结构;与体相g-C₃N₄（BCN）和3D g-C₃N₄相比,复合光催化剂有着更好的可见光吸收能力。以三乙醇胺为牺牲剂,在波长λ≥420 nm的可见光下进行产氢试验,研究了3D g-C₃N₄/Ni_xP复合光催化剂的光催化性能。结果表明,光沉积20 min得到的3D g-C₃N₄/Ni_xP复合光催化剂的光催化产氢速率可达1 720 μmol/（g·h）,远远大于纯DCN（7 μmol/（g·h））和光沉积20 min得到的BCN/Ni_xP复合光催化剂（15 μmol/（g·h））,并且在经历5个光催化循环产氢测试后其循环性能没有明显降低。     

碳掺杂TiO_2光催化剂处理有机污染物的研究

本文利用自制的碳掺杂改性TiO2光催化剂对甲基橙的光催化降解进行了研究,探索了光催化剂的最佳活性条件.实验表明：催化剂在350℃下焙烧4 h,且负载量为3∶2时光催化活性最佳;当催化剂用量为0.3 g时,光照0.5 h甲基橙的降解率为99%以上;当双氧水用量为2 mL时光催化剂催化活性最高,同时比较了紫外光下和太阳光下降解效果,显然太阳光下效果远远差于紫外光下的降解效果,但催化剂已经向可见光吸收范围转移.     

非TiO2可见光响应半导体氧化物光催化研究进展

继TiO2光催化剂以后的第二代光催化剂-可见光光催化剂由于可以直接利用太阳光对污染物进行降解,甚至可以分解水产生氢能,而成为当今环境领域的研究热点.本文综述了近年来非TiO2可见光响应的氧化物催化剂的研究现状,包括金属氧化物、复合氧化物、杂多酸、卤氧化物的研究进展;概述了其氧化物的制备方法、光催化特性及机理;最后对其氧化物可见光光催化研究进行了展望.     

异质结构钒酸铋/氧化铋可见光催化材料的制备及性能研究

针对可见光催化材料大部分半导体光量子效率较低、光催化活性较差的问题,制备了一种新的异质结构钒酸铋/氧化铋可见光催化材料,并对其性能进行测试。通过制备钒酸铋-氧化铋复合光催化材料,分析制备材料表征分析方法,对可见光催化材料进行XDR分析、SEM分析、紫外-可见漫反射吸收光谱分析和荧光光谱分析,对制备材料降解性能和稳定性进行检测。结果表明XDR分析中,随着钒酸铋成分的逐渐升高,氧化铋衍射峰慢慢降低,钒酸铋衍射峰慢慢增强,图谱中没有出现其余衍射峰,钒酸铋和氧化铋间未出现显著的化学反应; SEM分析中,制备样本颗粒形貌与微观结构存在显著差异,晶粒形貌更加规则;紫外-可见漫反射吸收光谱分析中,异质结构钒酸铋/氧化铋可见光催化材料样本对可见光的吸收效果最优;荧光光谱分析中,随着添加钒酸铋质量分数的逐渐增加,荧光信号逐渐变弱;随着添加钒酸铋质量分数的逐渐增加,降解率逐渐升高,但添加质量分数是12%与20%钒酸铋的制备样本光催化活性相差不大;重复使用制备样本后其光催化性能基本没有发生改变,对光照反应后制备样本及纯钒酸铋样本进行XRD分析,发现无新衍射峰值出现。可见此时制备样本降解性能较强,稳定性较高。     

复合铌酸盐的合成和光催化活性的研究

利用光催化剂降解有机染料具有很好的应用前景,光催化材料在光催化反应中起着重要的作用,但是如何制备化学性质稳定、在可见光下具有高的催化活性的催化剂一直是人们探索的一个主题。以Ag2O、Nb2O5、Na2CO3为前驱物,经高温固相反应法合成了具有不同Na/Ag摩尔比的(AgNbO3)1-x(NaNbO3)x复合铌酸盐。采用X-射线粉末衍射(XRD)、紫外-可见漫反射谱(UV-vis DRS)等方法对样品的结构和光谱响应特征进行了表征,以亚甲基蓝的降解反应为探针考察不同Na/Ag摩尔比的(AgNbO3)1-x(NaNbO3)x复合铌酸盐在可见光下的光催化活性。结果表明,由高温固相法合成出的复合铌酸盐的结构随着Na/Ag摩尔比的变化而变化,光谱响应特征随Na/Ag摩尔比的减小逐渐红移,而对亚甲基蓝的降解性能随Na/Ag呈规律性变化,其中(AgNbO3)0.6(NaNbO3)0.4复合铌酸盐呈现最好的光催化活性。     

Bionic titania coating carbon multi-layer material derived from natural leaf and its superior photocatalytic performance

Bionic titania coating carbon multi-layer material was fabricated by employing canna leaves as substrate and carbon precursor. Titania nanocrystals were assembled and coated on the natural films. The carbonation treatment under pure N_2 atmosphere yielded the ultrathin multi-film hybrid material. The carbon layer was coated with small anatase titania crystallite(8–10 nm) and possessed a highly specific surface area of 248.3 m~2 g~(-1). Examination using UV–visible spectrophotometer(UV–vis) showed that the band gap of the multi-layer material was reduced to 2.75 eV, and the hydrogen production by photocatalytic splitting of water under visible light irradiation was about 302 μmol g~(-1) after six hour.     

高能球磨制备MgxTi100-x合金的微观组织及储氢性能

应用振动高能球磨机械合金化方法制备MgxTi100-x(x=35,50,65,80)系列合金,采用XRD、SEM、TEM以及吸放氢测试等手段分析研究Mg含量与球磨时间对MgxTi100-x球磨产物微观组织演化规律、相结构和吸氢行为的影响.结果表明:在相同球磨时间(20 h)下,球磨合金MgxTi100-x微观组织的相组...