纳米FeVO_4的制备及其可见光下降解甲苯的性能

以Fe(NO3)3或FeCl3作为铁源,采用水热法制备了纳米FeVO4光催化剂,通过XRD、SEM、DRS等手段表征了所合成FeVO4的物相、表面形貌及光学性质,研究了其可见光下光催化降解甲苯的性能。表征结果显示:FeVO4平均晶粒尺寸约为75 nm,为棒状;FeVO4在可见光区域(λ400 nm)表现出较高的吸光性,其吸光区域可红移至约600 nm;以FeCl3为铁源,水热反应3 h制备的FeVO4的禁带宽度为2.1 e V;以Fe(NO3)3为铁源制备的FeVO4的比表面积(74.70 m2/g)大于以FeCl3为铁源制备的FeVO4的比表面积(67.72 m2/g)。在初始甲苯质量浓度为494 mg/L、FeVO4为光催化剂、反应4 h的条件下,甲苯降解率达62%。甲苯降解最终产物为CO2和H2O。     

电气石球负载纳米二氧化钛光催化剂的制备及其对水中邻苯二甲酸酯的降解作用

以电气石微球为载体,采用溶胶–凝胶法制备电气石负载纳米二氧化钛(TiO_2)光催化材料。用X射线衍射分析、扫描电镜对微球负载TiO_2光催化剂的晶型结构和形貌进行了表征。以6种邻苯二甲酸酯为降解对象,考察了热处理温度、辐射强度对TiO_2光催化活性的影响。发现TiO_2以纳米颗粒的形式牢固负载在电气石微球表面;以天然电气石微球为载体所制得的TiO_2光催化剂对于6种邻苯二甲酸酯具有较好的光催化降解效果。     

TiO2晶体的微波水热法制备及光催化性能研究

以TiSO4和尿素为主要原料,EDTA为控制剂,采用微波水热法制备纳米TiO2光催化剂,并分析了纳米TiO2晶粒的最佳形成条件。利用XRD、TEM等技术对制备产物进行表征。结果表明,TiSO4和尿素混合物在微波水热条件下晶化150min后,产物为锐钛矿型TiO2,且产物粒径小、大小均匀。在紫外光照射下,以自制的锐钛矿型纳米TiO2为催化剂,酸性橙为降解目标物,进一步研究了其光催化性能。结果表明,该TiO2在紫外光照射下表现出稳定的光催化活性。     

具有可见光活性的氮掺杂TiO2光催化剂的制备及光催化性能

采用浓氨水处理Ti(SO4)2溶液,然后经过滤、干燥、煅烧制备了一种氮掺杂TiO2光催化剂TiO2-XNX,其最佳煅烧温度为400℃。对该光催化剂的XRD谱图进行分析,结果表明,TiO2-XNX的晶型为锐钛矿相。紫外—可见吸收光谱表明,该光催化剂在可见光区具有明显的吸收。甲基橙溶液的降解实验结果表明,制备的TiO2-XNX光催化剂具有可见光(波长λ400nm)活性。     

BiOCl-(NH4)3PW12O40复合光催化剂制备及其光催化降解污染物机制

光生电子和空穴的分离效率是影响光催化性能的重要因素.氯氧铋是典型的层状纳米光催化剂,却因光生电子和空穴的快速复合所表现出的低量子效率而受到使用限制.本文通过两步的水热法合成了BiOCl-(NH_4)_3PW_(12)O_(40)复合光催化剂.以甲基橙(MO)为模拟污染物进行光催化活性测试.结果表明,在氙灯模拟的太阳光照射下,Bi与W的原子比为1∶1时,其催化效果最佳.通过自由基猝灭实验对催化剂光降解MO的催化机制进行了研究,发现BiOCl是由空穴,羟基自由基和超氧自由基共同作用来对MO进行降解;而复合催化剂则主要以羟基自由基和超氧自由基为活性物种来降解MO.通过对反应前后的催化剂进行XPS分析,证明了磷钨酸铵可以接收BiOCl产生的光生电子.通过光电流测试,表明复合光催化剂的光生电子的转移和分离效率有了较大的提高,从而提高了光催化活性.     

One-step synthesis of N-doped metal/biochar composite using NH3-ambiance pyrolysis for efficient degradation and mineralization of Methylene Blue

A series of new biochar-supported composite based on the combination of biochar and metallic nanoparticles(NPs)were produced through single-step pyrolysis of FeCl_3–Ti(OBu)_4 laden agar biomass under NH_3 environment.The physiochemical properties of composites were characterized thoroughly.It has found that heating temperature and N-doping through NH_3-ambiance pyrolysis significantly influence the visible-light sensitivity and bandgap energy of composites.The catalytic activities of composites were measured by degradation of Methylene Blue(MB)in the presence or absence of H_2O_2 and visible-light irradiation.Our best catalyst(N–TiO_2–Fe_3O_4-biochar)exhibits rapid and high MB removal competency(99.99%)via synergism of adsorption,photodegradation,and Fenton-like reaction.Continuous production of O_2U~-and UOH radicles performs MB degradation and mineralization,confirmed by scavenging experiments and degradation product analysis.The local trap state Ti~(3+),Fe_3O_4,and N-carbon of the catalyst acted as active sites.It has suggested that the Ti~(3+)and N-doped dense carbon layer improve charge separation and shuttle that prolonged photo-Fenton like reaction.Moreover,the catalyst is highly stable,collectible,and recyclable up to 5 cycles with high MB degradation efficiency.This work provides a new insight into the synthesis of highly visible-light sensitized biocharsupported photocatalyst through NH_3-ambiance pyrolysis of NPs-laden biomass.     

Cu2O-Ag-AgBr/MA可见光催化剂的制备及其降解2-氯苯酚的研究

通过沉积-沉淀法将Cu2O、Ag-AgBr负载在介孔γ-Al2O3(MA)上制备了等离子体诱导可见光催化剂Cu2O-Ag-AgBr/MA.研究了其在可见光照(λ>420 nm)下的催化性能.通过XRD、XPS和UV-vis吸收光谱的去卷积分析表明,表面银以Ag+和Ag0形式共存.结果表明,Cu2O-Ag-AgBr/MA对难降解有机物2-氯苯酚(2-CP)显示出很高的可见光催化去除效率.同时Cu2O的掺入,显著抑制了降解过程中Ag+的溶出.自由基捕获剂的影响实验表明,h+、O·-2和·OH是反应中最重要的活性物种.     

Fe/TiO2/ACF三元复合光催化材料联合脉冲放电降解甲基橙

采用溶胶-凝胶法制备了Fe/TiO₂/ACF三元复合光催化材料,将其投入到脉冲放电水处理反应器中降解甲基橙,考察该材料的光催化性能,以及它与脉冲放电的联合降解过程中操作因素的影响. 结果表明,Fe/TiO₂/ACF三元复合光催化材料与脉冲放电产生协同作用,大大提高了对甲基橙的去除率. 甲基橙的去除率与掺铁量〔以摩尔分数计〕、煅烧温度、溶液电导率和pH有关. 当掺铁量为0.07%,煅烧温度为900 ℃时,降解效果最佳;当溶液pH为6,电导率为300 μS/cm时,对Fe/TiO₂/ACF与脉冲放电的联合降解效果有利.      

氮化碳增强Ag/AgI/γ-Al2O3的可见光催化性能及其机理

通过热聚合的方法使氮化碳(CN)与Ag/AgI/γ-Al_2O_3发生耦合作用,制备出CN-Ag/AgI/γ-Al_2O_3可见光催化剂.采用X射线衍射(XRD)、X射线光电子能谱(XPS)、透射电子显微镜(TEM)和紫外可见漫反射光谱(UV-vis DRS)等方法对合成的样品进行了表征,并通过可见光下甲基橙(MO)的降解实验探究了CN对Ag/AgI/γ-Al_2O_3光催化活性及稳定性的影响.结果表明,CN的掺杂改变了Ag纳米颗粒的形状与粒径,且Ag、AgI与CN之间形成强相互作用.与Ag/AgI/γ-Al_2O_3相比较,在可见光波长分别为λ420、450和510 nm时,CN-Ag/AgI/γ-Al_2O_3对MO具有更高的催化降解效率,光反应30 min后,MO的去除率分别为97%、97%和93%.同时,CN的加入显著地增加了Ag/AgI/γ-Al_2O_3的稳定性,抑制了反应过程中Ag~+的释放量,而且反应前后CN-Ag/AgI/γ-Al_2O_3样品的结构没有明显的变化.其活性和稳定性提高的主要原因是CN加速了电子由MO传递至Ag纳米颗粒的过程,同时Ag颗粒等离子体共振(plasmon)效应的增强也有利于MO的催化降解.不同自由基捕获剂的影响实验表明,O_2~(·-)和h~+是反应体系的主要活性物种.     

Graphitic carbon nitride-based photocatalysts in the applications of environmental catalysis

Semiconductor photocatalytic technology has shown great prospects in converting solar energy into chemical energy to mitigate energy crisis and solve environmental pollution problems. The key issue is the development of high-efficiency photocatalysts. Various strategies in the state-of-the-art advancements, such as heterostructure construction, heteroatom doping, metal/single atom loading, and defect engineering, have been presented for the graphitic carbon nitride (g-C₃N₄)-based nanocomposite catalysts to design their surface chemical environments and internal electronic structures to make them more suitable for different photocatalytic applications. In this review, nanoarchitecture design, synthesis methods, photochemical properties, potential photocatalytic applications, and related reaction mechanisms of the modified high-efficiency carbon nitride-based photocatalysts were briefly summarized. The superior photocatalytic performance was identified to be associated with the enhanced visible-light response, fast photoinduced electron-hole separation, efficient charge migration, and increased unsaturated active sites. Moreover, the further advance of the visible-light harvesting and solar-to-energy conversions are proposed.