共查询到20条相似文献,搜索用时 31 毫秒
1.
采用水热方法制备了ZnIn2S4/g-C3N4复合材料, 并通过X射线衍射(XRD)、 傅里叶变换红外光谱(FTIR)、 紫外-可见漫反射光谱(UV-Vis DRS)、 透射电子显微镜(TEM)和荧光光谱(PL)等手段对其结构和性能进行表征. 结果表明, 当ZnIn2S4的负载量为20%(质量分数)时, 复合材料表现出最佳的光催化制氢性能, 制氢速率可达到637.08 μmol·g-1·h-1, 分别为纯ZnIn2S4和纯g-C3N4的4倍和37倍. 其原因在于ZnIn2S4和g-C3N4之间具有紧密的异质结结构, 两者有效的结合改善了组分的能带匹配和界面电荷转移, 从而大幅增强了载流子的分离和迁移, 进而提高光催化的性能. 相似文献
2.
纳米片与空心球上之间的合理界面调控是开发高效太阳能制氢光催化剂的潜在策略。在各类光催化材料中,金属硫化物由于具有相对较窄的带隙和优越的可见光响应能力而被广泛研究。ZnIn2S4是一种层状的三元过渡金属半导体光催化剂,其带隙可控(约2.4 eV)。在众多金属硫化物光催化剂中,ZnIn2S4引起了广泛兴趣。然而,单纯的ZnIn2S4光催化活性仍然相对较差,主要是因为光生载流子的复合率较高、迁移速率较慢。在半导体光催化剂上负载助催化剂是提升光催化剂性能的一种有效方法,因为它不仅可以加速光生电子和空穴的分离,而且还可以降低质子还原反应的活化能。作为一种三元过渡金属硫化物,NiCo2S4表现出较高的导电性、较低的电负性、丰富的氧化还原特性以及优越的电催化活性。这些特性表明,NiCo2S4可以作为光催化制氢的助催化剂,以加速电荷分离和转移。此外,NiCo2S4和ZnIn2S4都属于三元尖晶石的晶体结构,这可能有助于构建具有紧密界面接触的NiCo2S4/ZnIn2S4复合物,从而提高光催化性能。本文中,将超薄ZnIn2S4纳米片原位生长到非贵金属助催化剂NiCo2S4空心球上,形成具有强耦合界面和可见光吸收的NiCo2S4@ZnIn2S4分级空心异质结构光催化剂。最优NiCo2S4@ZnIn2S4复合样品(NiCo2S4含量:ca. 3.1%)的析氢速率高达78 μmol·h-1,约是纳米片组装ZnIn2S4光催化剂析氢速率的9倍、约是1% (w, 质量分数)Pt/ZnIn2S4样品析氢速率的3倍。此外,该复合光催化剂在反应中表现出良好的稳定性。荧光和电化学测试结果表明,NiCo2S4空心球是一种有效的助催化剂,可促进光生载流子的分离和传输,并降低析氢反应的活化能。最后,提出了NiCo2S4@ZnIn2S4光催化析氢的可能反应机理。在NiCo2S4@ZnIn2S4复合光催化剂中,具有高导电性的NiCo2S4助催化剂可快速接受ZnIn2S4上的光生电子,用以还原质子生成氢气,而电子牺牲剂TEOA捕获光生空穴,进而完成光催化氧化还原循环。该研究有望为基于纳米片为次级结构的分级空心异质结光催化剂的设计合成及其光催化制氢研究提供一定的指导。 相似文献
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通过水热和原位还原法制备了一种新型Z型异质结三元复合材料Au NPs/g-C3N4/BiOBr,并通过X射线衍射、X射线光电子能谱、透射电子显微镜、紫外-可见漫反射光谱和光致发光发射光谱等技术对材料的形貌、结构进行了表征。通过在可见光下降解苯酚来评价光催化剂的活性。研究发现,Au NPs/g-C3N4/BiOBr显示出增强的光催化活性,对苯酚的降解能力是g-C3N4的3倍,是BiOBr的2.5倍。这可归因于三元复合材料的窄带隙(2.10eV)、Z型机理对光生电子-空穴对的有效分离和Au纳米颗粒的表面等离子体共振效应(SPR)。 相似文献
4.
通过简单溶剂热法制备了一种新型复合光催化剂BiVO_4/M IL-53(Fe);运用XRD、SEM/EDS、FT-IR、N_2吸附-脱附和UV-vis DRS等手段对其进行表征,并对其光催化降解RhB活性进行了研究,提出了相应的光催化降解RhB的可能机理。结果表明,相较于单一BiVO_4材料,复合催化剂的比表面积增大,且其光催化效率相较于纯BiVO_4和MIL-53(Fe)也有了较大的提高;其中,BF-2复合材料的光催化活性最高,分别约为纯MIL-53 (Fe)和BiVO_4的5. 2倍和8. 1倍。同时,BiVO_4/MIL-53(Fe)复合光催化剂经过四次循环实验后,仍能保持较稳定的光催化活性和结构。 相似文献
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Due to the quite sluggish charge-carrier separation in semiconductor photocatalysts, the photocatalytic activity of these materials is still far inferior than anticipated. Herein, a novel approach to reducing the packing factor(PF) of ZnIn2S4 semiconductors to improve the charge-carrier separation is offered. The well-crystallized Zn1-xIn2S4-x(x=0, 0.05, 0.1) powders were productively prepared through solid-state reactions. Their structures were verified by the high-resolution transmission electron microscopy, powder X-ray diffraction, and X-ray photoelectron spectroscopy. The PF values of Zn1-xIn2S4-x(x=0, 0.05, 0.1) samples were calculated to be 0.683, 0.651, and 0.618, respectively. The reduction of the PF for Zn1-xIn2S4-x with increasing x can promote the separation of photoexcited carriers, and this process was endorsed by their photoelectric response and photoluminescence emission spectra. The Zn0.9In2S3.9 sample with a lower PF value presents roughly 21 times higher photocurrent density and four times higher photodegrading rate of methyl orange than those of pristine ZnIn2S4. 相似文献
6.
Yiqing Feng Hanyun Cheng Jin Han Xiuzhen Zheng Yangyang Liu Yang Yang Liwu Zhang 《中国化学快报》2017,28(12):2254-2258
Converting solar energy into valuable hydrogen and hydrocarbon fuels through photoelectrocatalytic water splitting and CO_2 reduction is highly promising in addressing the growing demand for renewable and clean energy resources. However, the solar-to-fuel conversion efficiency is still very low due to limited light absorption and rapid bulk recombination of charge carriers. In this work, we present chlorophyll(Chl) and its derivative sodium copper chlorophyllin(ChlCuNa), as dye sensitizers, modified BiVO_4 to improve the photoelectrochemical(PEC) performance. The photocurrent of BiVO_4 is surprisingly decreased after a direct sensitization of Chl while the sensitization of ChlCuNa obviously enhances photocurrent of BiV04 electrodes by improved surface hydrophilicity and extended light absorption.ChlCuNa-sensitized BiV04 achieves an improved H_2 evolution rate of 5.43 μmol h~(-1) cm~(-2) in water splitting and an enhanced HCOOH production rate of 2.15 μmol h~(-1) cm~(-2) in CO_2 PEC reduction, which are1.9 times and 2.4 times higher than pristine BiVO_4, respectively. It is suggested that the derivative ChlCuNa is a more effective sensitizer for solar-to-fuel energy conversion and CO_2 utilization than Chl. 相似文献
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8.
The threat and global concern of energy crises have significantly increased over the last two decades. Because solar light and water are abundant on earth, photocatalytic hydrogen evolution through water splitting has been considered as a promising route to produce green energy. Therefore, semiconductor photocatalysts play a key role in transforming sunlight and water to hydrogen energy. To date, various photocatalysts have been studied. Among them, TiO2 has been extensively investigated because of its non-toxicity, high chemical stability, controllable morphology, and high photocatalytic activity. In particular, 1D TiO2 nanofibers (NFs) have attracted increasing attention as effective photocatalysts because of their unique 1D electron transfer pathway, high adsorption capacity, and high photoinduced electron–hole pair transfer capability. However, TiO2 NFs are considered as an inefficient photocatalyst for the hydrogen evolution reaction (HER) because of their disadvantages such as a large band gap (~3.2 eV) and fast recombination of photoinduced electron–hole pairs. Therefore, the development of a high-performance TiO2 NF photocatalyst is required for efficient solar light conversion. In recent years, several strategies have been explored to improve the photocatalytic activity of TiO2 NFs, including coupling with narrow-bandgap semiconductors (such as ZnIn2S4). Recently, microwave (MW)-assisted synthesis has been considered as an important strategy for the preparation of photocatalyst semiconductors because of its low cost, environment-friendliness, simplicity, and high reaction rate. Herein, to overcome the above-mentioned limiting properties of TiO2 NFs, we report a 2D/1D ZnIn2S4/TiO2 S-scheme heterojunction synthesized through a microwave (MW)-assisted process. Herein, the 2D/1D ZnIn2S4/TiO2 S-scheme heterojunction was constructed rapidly by using in situ 2D ZnIn2S4nanosheets decorated on 1D TiO2 NFs. The loading of ZnIn2S4 nanoplates on the TiO2 NFs could be easily controlled by adjusting the molar ratios of ZnIn2S4 precursors to TiO2 NFs. The photocatalytic activity of the as-prepared samples for water splitting under simulated solar light irradiation was assessed. The experimental results showed that the photocatalytic performance of the ZnIn2S4/TiO2 composites was significantly improved, and the obtained ZnIn2S4/TiO2 composites showed increased optical absorption. Under optimal conditions, the highest HER rate of the ZT-0.5 (molar ratio of ZnIn2S4/TiO2= 0.5) sample was 8774 μmol·g-1·h-1, which is considerably higher than those of pure TiO2 NFs (3312 μmol·g-1·h-1) and ZnIn2S4nanoplates (3114 μmol·g-1·h-1) by factors of 2.7 and 2.8, respectively. Based on the experimental data and Mott-Schottky analysis, a possible mechanism for the formation of the S-scheme heterojunction between ZnIn2S4 and TiO2 was proposed to interpret the enhanced HER activity of the ZnIn2S4/TiO2heterojunctionphotocatalysts.
相似文献
9.
以硝酸铋为铋源,偏钒酸铵为钒源,醋酸钠调节pH值,采用水热法合成光催化剂BiVO_(4),采用X-射线衍射仪(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)对产物进行结构和形貌分析.在可见光条件下,考察BiVO_(4)对甲基橙(MO)的光催化性能.结果表明,在pH值为6.0的条件下合成的BiVO_(4)具有较优的光催化性能,可见光条件下催化反应5 h后,MO的降解率达到98.4%,并且在循环反应5次后对MO的降解率仍在95%以上.因BiVO_(4)良好的光催化活性和稳定性,在废水处理领域有非常广阔的应用前景. 相似文献
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基于类十面体钒酸铋(BiVO4)和氧化铜(CuO)纳米颗粒, 构筑了CuO/BiVO4异质结光催化剂; 利用X射线衍射仪(XRD)、 X射线光电子能谱仪(XPS)、 扫描电子显微镜(SEM)、 紫外-可见吸收光谱(UV-Vis)、 光电流响应谱(I-t)、 电化学阻抗谱(EIS)和荧光发射光谱(PL)对催化剂的形貌、 结构和光电性能进行了表征和分析. 结果表明, CuO纳米颗粒均匀地负载在BiVO4的表面, 通过控制铜源的用量可以调节CuO的含量, 其含量对CuO/ BiVO4异质结的可见光吸收能力和光生载流子的分离效率有很大的影响. 在气固反应体系下, 对CuO/BiVO4异质结的光催化还原CO2的性能进行了研究. 结果显示, 光催化还原CO2的主要产物为CO和CH4; 随着CuO含量的增加, CO的产率逐渐降低, 而CH4的产率先增加后降低, 最优化催化剂CuO/BiVO4的CO和CH4的产率分别为0.62和1.81 μmol·g-1·h-1, 对CH4的选择性达到最大值(93%). 能带结构分析和电子顺磁共振(EPR)测试结果表明, CuO/BiVO4中光生电荷的转移符合Z型转移机制. Z型异质结构的形成, 促进了光生电子和空穴的分离, 提升了催化体系的氧化还原能力. 相似文献
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通过金属有机物分解法(MOD)协同光电化学沉积法, 将p型氧化物半导体CuBi2O4沉积在BiVO4纳米薄膜上, 形成包覆性异质结结构, 制备了一种新型p-n异质结光阳极n-BiVO4/p-CuBi2O4, 用于太阳能光电化学(Photoelectrochemical, PEC)水分解. 研究结果表明, 在1.23 V(vs. RHE)电势下, BiVO4/CuBi2O4 异质结光阳极表现出优良的PEC水氧化性能, 光电流密度达到2.8 mA/cm2, 负载磷酸钴(Co-Pi)的BiVO4/CuBi2O4/Co-Pi光电极, 光电流密度达到4.45 mA/cm2, 分别为BiVO4电极光电流密度的3.1倍和4.9倍. X射线衍射(XRD)、 紫外-可见吸收光谱(UV-Vis)、 电化学阻抗谱(EIS)和能级结构图等结果也证实, BiVO4/CuBi2O4和BiVO4/CuBi2O4/Co-Pi复合电极材料在内建电场和能带弯曲作用下, 光吸收特性增强, 载流子界面转移电阻减小, 具有良好的光电化学性能与稳定性. 相似文献
12.
A PEC cell with nanostructured BiVO4 photoelectrode film presents outstanding azo dye degradation and simultaneous H2 production performance. 相似文献
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采用一步水热法制备Bi2MoO6/BiVO4复合光催化剂.利用X射线衍射(XRD)、场发射扫描电子显微镜(FESEM)、高分辨透射电子显微镜(HRTEM)等手段对其晶体结构和微观结构进行了表征.结果表明,Bi2MoO6纳米粒子沉积在BiVO4纳米片表面从而形成异质结结构.紫外-可见漫反射光谱(UV-Vis DRS)表明所制备的Bi2MoO6/BiVO4异质结较纯相Bi2MoO6和BiVO4对可见光吸收更强.由于形成异质结结构及其光吸收性能使Bi2MoO6/BiVO4光催化活性有较大提高.可见光下(λ420 nm)光催化降解罗丹明B(RhB)实验结果表明,Bi2MoO6/BiVO4光催化活性较纯相Bi2MoO6和BiVO4高.Bi2MoO6/BiVO4样品光催化性能提高的原因是Bi2MoO6和BiVO4形成异质结,从而有效抑制光生电子-空穴对的复合,增大了可见光吸收范围及比表面积. 相似文献
14.
Meng Ding Juanjuan Zhou Hongcen Yang Ruya Cao Shouwei Zhang Minghui Shao Xijin Xu 《中国化学快报》2020,31(1):71-76
Graphene-like C3N4/Ag3PO4 photocatalysts are synthesized by calcination and solutions precipitating method.The obtained g-C3N4/Ag3PO4 composites display excellent photocatalytic activity for the degradation of methylene orange(MO),rhodamine B(RhB)and tetracycline(TC)under visible light irradiation.The solutions containing RhB(10 mg/L)and MO(10 mg/L)can be efficiently degraded within15 min and 30 min.Especially,nearly 80%of TC(50 mg/L)is degraded within 20 min.which are much better than those of pure g-C3N4 nanosheets and Ag3PO4,implying that strong interaction and reasonable energy band alignment in the contact interface can effectively transfer the carries.Furthermore,the g-C3N4/Ag3PO4 composites exhibit the improved stability,and only a slight decrease is observed after three recycling runs.Moreover,the impact of inorganic ions and PH values on the degradation performance is rather small.The Z-scheme photocatalytic mechanism of the g-C3N4/Ag3PO4 composites based on the active species trapping experimental is proposed.This work demonstrates the promising applications of the g-C3N4/Ag3PO4 composites in environmental issues. 相似文献
15.
用简单的超声分散法合成了具有可见光响应的类石墨氮化碳(g-C3N4)/BiVO4复合光催化剂. 采用X射线衍射(XRD), X射线光电子能谱(XPS), 扫描电子显微镜(SEM), 透射电子显微镜(TEM), 紫外-可见(UV-Vis)分光光谱, 傅里叶红外变换(FTIR)光谱, 荧光发射谱(PL)和光电流响应等技术对所制备催化剂进行相关表征. 通过可见光下(λ> 420 nm)光催化还原CO2的性能来评价样品的光催化活性, 发现不同复合比的催化剂中, 含40% (w) g-C3N4的复合催化剂表现出最高的光催化活性, 其催化活性分别为纯g-C3N4纳米片和纯BiVO4的催化活性的2倍和4倍.光催化活性增加的主要原因是g-C3N4和BiVO4之间形成了异质结, 且相互间能级匹配, 有利于光生电子和空穴的分离. 相似文献
16.
全球工业化进程的加快使人们饱受环境污染问题的困扰.半导体光催化技术作为一种高效、绿色、有潜力的新技术,在环境净化方面有着广阔的应用前景.Bi2O4是近年来新开发出的一种铋基光催化剂,在环境净化方面已有一些研究.但是,单体光催化剂通常存在光响应范围窄、光生载流子复合率高等问题,这些不足限制了Bi2O4的进一步应用.因此,需要通过适当的改性来拓宽其光响应范围和提高其载流子的分离效率,从而提高其光催化活性.构建Z型异质结被认为是提高光催化剂光生载流子分离效率并进一步提高光催化活性的有效方法.MoO3是一种宽禁带的n型半导体,具有独特的能带结构、光学特性和表面效应,是一种非常有前景的半导体光催化剂.虽然MoO3材料的光生载流子复合率高,带隙(2.7-3.2 eV)大,不利于其参与光催化反应,但MoO3与其他合适的半导体配位形成复合材料后能够有效提高其光生载流子的分离效率,从而提高其光催化活性.本研究采用简单的水热法制备了一种新型Z型MoO3/Bi2O4复合光催化剂,SEM和TEM分析结果表明,MoO3和Bi2O4紧密结合在一起.X射线光电子能谱分析表明,MoO3和Bi2O4之间存在很强的界面相互作用,这有助于电荷转移和光生载流子的分离.光致发光光谱、电阻抗和光电流测试也证明了MoO3/Bi2O4复合光催化剂的光生载流子分离效率更高,形成了更强的光电流.通过在可见光下降解RhB溶液评价了所合成光催化剂的光催化性能.15%MoO3/Bi2O4(15-MB)复合光催化剂表现出了最佳的可见光催化活性,在40 min内对10 mg/L RhB溶液的降解率达到了99.6%,其降解速率是Bi2O4的2倍.此外,15-MB复合光催化剂在经过五次循环降解RhB溶液后仍保持良好的光催化活性和稳定性,表明MoO3/Bi2O4复合光催化剂具有较强的应用潜力.通过自由基捕获实验确定了光催化反应中主要的活性自由基为 O2-和h+.通过莫特-肖特基测试和带隙计算得到MoO3和Bi2O4的价带和导带位置.最后,根据实验和分析结果提出了Z型MoO3/Bi2O4复合光催化剂在可见光下降解RhB溶液的机理.本研究为设计铋基Z型异质结光催化剂用于高效去除环境污染物提供了一种有前景的策略. 相似文献
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采用水热后合成法制备了BiVO_4/SBA-15催化剂,利用XRD、SEM-EDS和N2吸附-脱附等手段对其进行表征分析,并在自制的光催化反应装置中对其静态光催化氧化脱硫性能进行了研究。结果表明,BiVO_4/SBA-15催化剂具有SBA-15分子筛的介孔孔道结构,BiVO_4均匀分布在SBA-15分子筛表面。BiVO_4/SBA-15催化剂具有良好的催化氧化脱硫性能,在BiVO_4负载量为15%、水热合成时间为18 h、530℃下焙烧3 h制备的BiVO_4/SBA-15催化剂,对模拟柴油的脱硫率可达95.6%。 相似文献
18.
采用水热法制备了ZnIn2S4固溶体, 并通过用盐酸对其进行后处理获得了系列ZnmIn2Sm+3(m≥2, 整数)固溶体. 通过X射线衍射(XRD)、 扫描电子显微镜(SEM)、 透射电子显微镜(TEM)、 X射线光电子能谱(XPS)、 紫外-可见漫反射光谱(UV-Vis DRS)、 荧光光谱(PL)和电化学测试对催化剂的组成、 结构和性能进行了表征. 研究了系列固溶体可见光光催化制氢活性. 结果表明, ZnIn2S4固溶体经0.5 mol/L HCl处理后能转化为Zn2In2S5固溶体, 其制氢活性为ZnIn2S4固溶体的2.2倍, 并且具有良好的稳定性. 相似文献
19.
结合回流法和原位沉淀法成功制备磷酸银/矾酸铋(Ag3PO4/BiVO4)复合光催化剂.通过X射线衍射(XRD)、场发射扫描电子显微镜(FESEM)、能量色散X射线光谱(EDS)、紫外-可见漫反射光谱(UV-Vis DRS)及光致发光(PL)光谱对制备样品进行表征.XRD和FESEM结果表明成功制备Ag3PO4/BiVO4复合光催化剂.采用节能发光二极管灯(LED)作为可见光光源,在低消耗光催化系统中评价制备样品可见光催化降解染料的活性.当Ag3PO4和BiVO4的组成摩尔比为1:3时,复合Ag3PO4/BiVO4光催化剂呈现出高于纯相Ag3PO4的催化活性,可减少Ag3PO4的使用量.Ag3PO4/BiVO4复合光催化剂在中性溶液中表现出高活性,同时证实其对阳离子染料的光催化降解效果强于阴离子染料.在Ag3PO4/BiVO4系统中,超氧自由基和空穴是主要的活性物种.经过三次循环利用,Ag3PO4/BiVO4复合催化剂的可见光催化活性表现出不同程度的降低,归因于降解过程中产生金属银. 相似文献
20.
CHEN Ting ZHONG Lei YANG Zhen MOU Zhigang LIU Lei WANG Yan SUN Jianhua LEI Weiwei 《高等学校化学研究》2020,36(6):1083-1090
Limited visible-light absorption and high recombination rate of photogenerated charges are two main drawbacks in g-C3N4-based photocatalysts. To solve these problems, g-C3N4/nitrogen-doped graphene quantum dots (NGQDs)/TiO2 ternary heterojunctions were facilely prepared via a one-step calcining method. The morphology, structure, optical and electrochemical properties of g-C3N4/NGQDs/TiO2 were characterized and explored. The optimal g-C3N4/NGQDs/TiO2 composite exhibits enhanced photocatalytic degradation performance of ciprofloxacin (CIP) compared with the as-prepared g-C3N4, TiO2(P25) and g-C3N4/TiO2 heterojunction under visible light irradiation. The apparent rate constant of the composite is around 6.43, 4.03 and 2.30 times higher than those of g-C3N4, TiO2 and g-C3N4/TiO2, respectively. The enhanced photocatalytic efficiency should be mainly attributed to the improvement of light absorption and charge separation and transfer efficiency, originating from the narrow band gap and high charge carrier mobility. The active species trapping experiments results showed that the h+ and ·O2- were the main active species in the degradation process. A possible photocatalytic reaction mechanism of the g-C3N4/NGQDs/TiO2 composite for the enhanced degradation of CIP under visible light irradiation was also proposed. 相似文献