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1.
With the rapid development of the world economy, water pollution has become increasingly serious. The photocatalytic degradation of pollutants is one of the most promising environmental treatment techniques. In this study, novel Ag3PW12O40/ZnO nanoheterojunction was successfully constructed via a chemical process and was then characterized using X-ray diffraction, transmission electron microscopy, scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, diffuse reflectance spectroscopy, Brunauer-Emmett-Teller analysis, and photoluminescence measurements. The synthesized nanoheterojunction exhibited good crystallinity and dispersity. The particle diameter of the composite was approximately 800 nm, the bandgap was 2.92 eV, and the specific surface area was approximately 10.5 m2.g?1. Under optimum conditions, the photocatalyst degraded 82.1% RhB in 60 min. Moreover, the novel Ag3PW12O40/ZnO heterojunction also exhibited an excellent recycling stability. Hydroxyl radicals, superoxide radicals, and holes played important roles in the photocatalytic degradation process. A possible mechanism for the enhanced photocatalytic performance of the nanoheterojunction was proposed. This work provides a strong foundation for the application of Ag3PW12O40/ZnO nanoheterojunction for treating environmental organic pollutants.  相似文献   

2.
The SrFe12O19/poly (vinyl pyrrolidone) (PVP) composite fiber precursors were prepared by the sol-gel assisted electrospinning with ferric nitrate, strontium nitrate and PVP as starting reagents. Subsequently, the M-type strontium ferrite (SrFe12O19) nanofibers were derived from calcination of these precursors at 750–1,000 °C.The composite precursors and strontium ferrite nanofibers were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy and vibrating sample magnetometer. The structural evolution process of strontium ferrite consists of the thermal decomposition and M-type strontium ferrite formation. After calcined at 750 °C for 2 h the single M-type strontium ferrite phase is formed by reactions of iron oxide and strontium oxide produced during the precursor decomposition process. The nanofiber morphology, diameter, crystallite size and grain morphology are mainly influenced by the calcination temperature and holding time. The SrFe12O19 nanofibers characterized with diameters of around 100 nm and a necklace-like structure obtained at 900 °C for 2 h, which is fabricated by nanosized particles about 60 nm with the plate-like morphology elongated in the preferred direction perpendicular to the c-axis, show the optimized magnetic property with saturation magnetization 59 A m2 kg−1 and coercivity 521 kA m−1. It is found that the single domain critical size for these M-type strontium ferrite nanofibers is around 60 nm.  相似文献   

3.
The composite nanofibers of xSrSiO3/(100 − x)SrFe12O19 (x = 0–13 wt%) with diameters around 110 nm have been prepared by calcination of the electrospun SrSiO3/SrFe12O19/poly (vinyl pyrrolidone) (PVP) composite fibers at 800–900 °C. The composite nanofibers were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy and vibrating sample magnetometer. After calcined at 800° the M-type strontium ferrite is formed and the strontium silicate exists as an amorphous state when the calcination temperature below about 950 °C. The addition of SrSiO3 has an obvious suppression effect on the strontium ferrite grain growth and the ferrite grain size decreases from 66.9 to 33.5 nm corresponding SrSiO3 content from 0 to 9 wt% in the composite. The specific saturation magnetization (Ms) of the xSrSiO3/(100 − x)SrFe12O19 composite nanofibers exhibits a continuous reduction from 58.0 to 45.6 A m2 kg−1 with the increase of SrSiO3 content from 0 to 13 wt%. With addition of SrSiO3 from 0 to 13 wt%, the coercivity of the composite nanofibers obtained at 900 °C initially increases, reaching a maximum value 501.1 kA m−1 at the silicate content 7 wt%, and then shows a reduction tendency with the strontium silicate content increase further up to 13 wt%. This influence on the coercivity by strontium silicate can be attributed mainly to the ferrite grain growth suppression and the non-magnetic phase barrier for the domains misalignment.  相似文献   

4.
采用水热法成功制备了MoS_2/WO3复合半导体光催化剂,分别通过SEM、TEM、EDS、XRD、Raman和DRS对催化剂的形貌,组成及结构进行表征,并用BET模型计算比表面积。对比发现球状MoS_2/WO3对罗丹明B(Rh B)的光降解效率明显高于纯WO3、片状MoS_2/WO3复合半导体。针对球状MoS_2/WO3复合半导体,分别研究了MoS_2不同负载量(0.5%,1%,2%,5%,10%)对Rh B光催化降解性能的影响,结果表明MoS_2含量为2%时催化效果最佳。同时,研究了溶液的p H值(p H=1,3,6,7,11)对光催化降解反应活性的影响,结果显示p H=6时降解率最高。当催化剂量增加到1 g·L-1时,30 min后Rh B降解率达到96.6%。球状MoS_2/WO3的瞬态光电流为0.050 6 m A·cm-2,比纯WO3提高了2.4倍。经过5次循环实验,球状MoS_2/WO3复合半导体催化剂仍能保持90%的高降解率。  相似文献   

5.
采用水热法成功制备了MoS2/WO3复合半导体光催化剂,分别通过SEM、TEM、EDS、XRD、Raman和DRS对催化剂的形貌,组成及结构进行表征,并用BET模型计算比表面积。对比发现球状MoS2/WO3对罗丹明B(RhB)的光降解效率明显高于纯WO3、片状MoS2/WO3复合半导体。针对球状MoS2/WO3复合半导体,分别研究了MoS2不同负载量(0.5%,1%,2%,5%,10%)对RhB光催化降解性能的影响,结果表明MoS2含量为2%时催化效果最佳。同时,研究了溶液的pH值(pH=1,3,6,7,11)对光催化降解反应活性的影响,结果显示pH=6时降解率最高。当催化剂量增加到1 g·L-1时,30min后RhB降解率达到96.6%。球状MoS2/WO3的瞬态光电流为0.050 6 mA·cm-2,比纯WO3提高了2.4倍。经过5次循环实验,球状MoS2/WO3复合半导体催化剂仍能保持90%的高降解率。  相似文献   

6.
《中国化学快报》2022,33(12):5200-5207
The matched energy band structure and efficient carrier separation efficiency are the keys to heterogeneous photocatalytic reactions. A novel organic/inorganic step scheme (S-scheme) heterojunction PDI-Urea/BiOBr composite photocatalyst was constructed by simple solvothermal reaction combined with in-situ growth strategy. The composite photocatalyst not only has high chemical stability, but also can generate and accumulate a large number of active species (h+, ?O2?, ?OH, H2O2). PDI-Urea/BiOBr showed higher photocatalytic activity for the degradation of antibiotic such as ofloxacin (OFLO), tetracycline (TC) and the production of H2O2 in the spectral range of 400–800 nm. The apparent rate constant of 15% PDI-Urea/BiOBr for photocatalytic degradation of TC (or OFLO) was 2.7 (or 2.5) times that of pure BiOBr and 1.7 (or 1.8) times that of pure PDI-Urea. The H2O2 evolution rate of 15% PDI-Urea/BiOBr was 2.5 times that of PDI-Urea and 1.5 times that of BiOBr, respectively. This work has formed a mature S-scheme heterojunction design thought and method, which offers new visions for the development of heterogeneous photocatalysts.  相似文献   

7.
随着全球工业化进程的发展,环境污染问题日益严重,已经成为21世纪影响人类生存与发展的重要问题.光催化氧化技术被认为是解决环境问题最有应用前景的技术之一,已经成为环境领域的研究热点.众所周知,二硫化钼(MoS2)可以被可见光激发产生电子-空穴对,但是由于其氧化还原电势并不高,抑制了氧分子活化的量子效率,且激发后的光生载流子容易复合,导致光催化效率不高.因此,迫切需要对MoS2光催化材料进行修饰与改性,采用提高光催化过程中活性氧(ROSs)的量来提高其光催化活性.银钒氧化物(AgVO3,Ag2V4O11,Ag3VO4和Ag4V2O7等)因其在锂电池、传感器和光催化剂领域的应用而引起了人们的关注.其中,AgVO3具有较窄的带隙和高度分散的价带,具有潜在的应用价值.本文采用水热法成功制备了AgVO3/MoS2复合光催化剂,并采用X射线粉末衍射、扫描电子显微、透射电子显微镜和紫外-可见漫反射光谱等表征技术研究了所制光催化剂的物相结构、样品形貌和光学性能.以四环素为研究对象,将其应用于AgVO3/MoS2复合光催化剂的降解实验.结果表明,随着AgVO3质量比从1.0 wt%增加到3.0 wt%,所得催化剂的光催化活性不断提高;当进一步增加AgVO3的质量时,复合催化剂的活性逐渐降低.这是由于过多的AgVO3的引入导致在光催化剂表面形成电子-空穴对复合中心,增加了载流子复合几率.因此,AgVO3/MoS2复合光催化剂中AgVO3的最佳质量比为3.0 wt%,其降解速率常数为0.0087 min–1,分别是MoS2(0.00509 min–1)和AgVO3(0.00495 min–1)的1.71和1.76倍.由于AgVO3改性后的MoS2具有优异的光催化性能,能促进O2的吸附/活化,加速MoS2表面生成H2O2的双电子氧还原反应,从而产生更多的ROSs.利用电子自旋共振光谱、POPHA荧光检测和自由基捕获实验相结合的方法来阐明ROSs的形成机理.同时,ROSs的产生会加速消耗AgOV3导带上的电子,为降解污染物留下更多的空穴.本文为表面催化工程促进ROSs生成的合理设计提供了新的思路,有望在环境治理中得到实际应用.  相似文献   

8.
通过焙烧-超声混合法成功地制备了BiOBr/g-C3N4S型异质结复合光催化剂。采用多种表征手段对样品物理属性进行了表征,包括X射线多晶粉末衍射仪(XRD)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)、紫外可见漫反射光谱(UV-Vis DRS)。研究了所制备样品有/无Fe3+的光-自芬顿催化/光催化降解罗丹明B(RhB)性能。通过捕获实验确定了光催化反应中的主要活性物种,提出了光-自芬顿反应的降解机理。研究结果表明,BiOBr/g-C3N4S型异质结能原位生成H2O2,添加Fe3+后,H2O2被原位活化成活性物种且光生电流和载流子分离效率获得显著提高。该光-自芬顿过程能高效降解RhB,其反应速率常数为0.208 min-1,约为无Fe3+光催化反应速率常数的5.3倍,在光-自芬顿循环使用过程中表现出良好的稳定性。Fe...  相似文献   

9.
In this study, we have introduced iodine into Bi4Ti3O12 (BTO) crystals with the aim of improving their photocatalytic activities in decomposing organic pollutants. The as-prepared Idoped-BTO photocatalysts were systematically analyzed by various techniques (e.g. X-ray powder diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, ultraviolet–visible diffuse reflectance spectroscopy and Fourier transform infrared spectroscopy), as well as density functional theory calculation. It is confirmed that I element is successfully doped, as an I? oxidation state, in the BTO crystals by substituting the O in the perovskite-like (Bi2Ti3O10)2? blocks. The photocatalytic activities between the Ix-BTO (x = 0, 0.2, 0.4, 0.6, and 0.8) samples were compared by the photodegradation of methylene blue (MB) under simulated-sunlight irradiation, revealing that I0.4-BTO is the optimal photocatalyst having a photocatalytic activity about 3.0 times higher than that of parent BTO. Based on the experimental data and density functional theory calculation, the enhanced photocatalytic mechanism for the Idoped-BTO photocatalysts was proposed and discussed. To promote the potential application of the optimal I0.4-BTO photocatalyst, its photocatalytic performances were further investigated by the photodegradation of ciprofloxacin, tetrabromobisphenol A, tetracycline hydrochloride and methyl orange/rhodamine B (RhB)/MB mixture dyes; moreover, the effect of inorganic anions and pH values on the MB photodegradation was also investigated.  相似文献   

10.
采用机械球磨法成功制备Ag3PO4/MoS2纳米片复合催化剂。运用X射线衍射仪(XRD)、透射电子显微镜(TEM)、扫描电子显微镜(SEM)、紫外可见漫反射光谱(UV-Vis)和荧光发射光谱(PL)对复合催化剂的结构和形貌进行了表征。结果表明,Ag3PO4纳米粒子均匀地附着在MoS2纳米片层结构上,两者形成紧密结合。以亚甲基蓝为模拟污染物,研究复合催化剂在可见光照射下的光催化特性;通过循环实验考察复合催化剂的稳定性。结果显示,含有1%的MoS2纳米片与Ag3PO4形成的复合催化剂在30 min内对亚甲基蓝的降解率为95%,其降解动力学常数是纯相Ag3PO4的2倍。经过5次循环实验后复合催化剂对于亚甲基蓝的降解率为84%,而纯Ag3PO4对于亚甲基蓝的降解率仅为35%。Ag3PO4/MoS2纳米片复合催化剂具有优良的光催化活性和高稳定性,主要归因于二硫化钼纳米片与磷酸银形成异质结,磷酸银激发的电子和二硫化钼纳米片产生的空穴直接复合,从而促使光生电子从磷酸银晶体表面快速分离,减轻了磷酸银的光电子腐蚀,同时也提高了复合物的光催化活性。  相似文献   

11.
采用机械球磨法成功制备Ag_3PO_4/MoS_2纳米片复合催化剂。运用X射线衍射仪(XRD)、透射电子显微镜(TEM)、扫描电子显微镜(SEM)、紫外可见漫反射光谱(UV-Vis)和荧光发射光谱(PL)对复合催化剂的结构和形貌进行了表征。结果表明,Ag_3PO_4纳米粒子均匀地附着在MoS_2纳米片层结构上,两者形成紧密结合。以亚甲基蓝为模拟污染物,研究复合催化剂在可见光照射下的光催化特性;通过循环实验考察复合催化剂的稳定性。结果显示,含有1%的MoS_2纳米片与Ag_3PO_4形成的复合催化剂在30 min内对亚甲基蓝的降解率为95%,其降解动力学常数是纯相Ag_3PO_4的2倍。经过5次循环实验后复合催化剂对于亚甲基蓝的降解率为84%,而纯Ag_3PO_4对于亚甲基蓝的降解率仅为35%。Ag_3PO_4/MoS_2纳米片复合催化剂具有优良的光催化活性和高稳定性,主要归因于二硫化钼纳米片与磷酸银形成异质结,磷酸银激发的电子和二硫化钼纳米片产生的空穴直接复合,从而促使光生电子从磷酸银晶体表面快速分离,减轻了磷酸银的光电子腐蚀,同时也提高了复合物的光催化活性。  相似文献   

12.
The RP/g-C3N4 heterojunction photocatalyst was fabricated by a facile heat treatment strategy. The obtained composite has excellent light harvesting ability and charge separation performance. Compared to single RP and g-C3N4, the 50%-RP/g-C3N4 exhibited enhanced photocatalytic activity for simultaneously removing Cr(VI) and RhB, and the removal rates can reach 92% and 99% in 25 min, respectively. The enhanced mechanism was revealed by active species capturing experiments, showing that electrons can reduce Cr(VI) and produce O2 in air and that holes can directly oxidize the dyes. The coexistence of Cr(VI) and RhB will lead to a synergistic improvement of Cr(VI) reduction and RhB degradation due to rapid surface reactions. This further improves the charge separation except for the heterojunction effect. In addition, the COD analysis demonstrates that organic dyes are mainly degraded into CO2, H2O and some intermediates.  相似文献   

13.
通过焙烧-超声混合法成功地制备了BiOBr/g-C3N4 S型异质结复合光催化剂。采用多种表征手段对样品物理属性进行了表征,包括X射线多晶粉末衍射仪(XRD)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)、紫外可见漫反射光谱(UV-VisDRS)。研究了所制备样品有/无Fe3+的光-自芬顿催化/光催化降解罗丹明B (RhB)性能。通过捕获实验确定了光催化反应中的主要活性物种,提出了光-自芬顿反应的降解机理。研究结果表明,BiOBr/g-C3N4 S型异质结能原位生成H2O2,添加Fe3+后,H2O2被原位活化成活性物种且光生电流和载流子分离效率获得显著提高。该光-自芬顿过程能高效降解RhB,其反应速率常数为0.208 min-1,约为无Fe3+光催化反应速率常数的5.3倍,在光-自芬顿循环使用过程中表现出良好的稳定性。Fe3+的加入促进了光生电荷的分离和H2O2的活化,超氧阴离子自由基(·O2-)、空穴和羟基是光-自芬顿催化过程中的主要活性物种,且·O2-作用更大。  相似文献   

14.
采用自组装和化学沉淀法分别制得两种可见光驱动复合材料石墨相氮化碳/碳酸氧铋(g-C_3N_4/Bi_2O_2CO_3).采用X射线衍射光谱(XRD),紫外可见光谱、扫描电镜(SEM)、N_2吸附、电化学阻抗谱(EIS)和X射线光电子能谱(XPS)等分析手段对制备的催化剂进行了表征.结果表明,制备方法对纳米复合材料的晶相、形态及光学性能没有影响,但是影响g-C_3N_4和Bi_2O_2CO_3之间的相互作用力,导致光生电子-空穴对的分离速率存在显著差异.以可见光驱动苯酚和罗丹明B的降解实验为探针反应检测催化剂的光催化性能.实验结果表明自组装法得到的异质结催化剂中相互作用力更强,催化效果最高.O_2-是罗丹明B降解反应的主要活性物种,染料的光敏化、Bi_2O_2CO_3与g-C_3N_4综合效应,导致光生载流子电荷分离效率更高.  相似文献   

15.
A novel graphene‐like MoS2/C3N4 (GL‐MoS2/C3N4) composite photocatalyst has been synthesized by a facile ethylene glycol (EG)‐assisted solvothermal method. The structure and morphology of this GL‐MoS2/C3N4 photocatalyst have been investigated by a wide range of characterization methods. The results showed that GL‐MoS2 was uniformly distributed on the surface of GL‐C3N4 forming a heterostructure. The obtained composite exhibited strong absorbing ability in the ultraviolet (UV) and visible regions. When irradiated with visible light, the composite photocatalyst showed high activity superior to those of the respective individual components GL‐MoS2 and GL‐C3N4 in the degradation of methyl orange. The enhanced photocatalytic activity of the composite may be attributed to the efficient separation of electron–hole pairs as a result of the matching band potentials between GL‐MoS2 and GL‐C3N4. Furthermore, a photocatalytic mechanism for the composite material has been proposed, and the photocatalytic reaction kinetics has been measured. Moreover, GL‐MoS2/C3N4 could serve as a novel sensor for trace amounts of Cu2+ since it exhibited good selectivity for Cu2+ detection in water.  相似文献   

16.
Exploring noble‐metal‐free, highly active and durable catalysts is vital to get to grips with the energy and environmental issues. Herein, we first dexterously design and synthesize a class of ternary Nb6/CZS/g‐CN photocatalysts for the removal of hexavalent chromium Cr (VI) and organic dye pollutant (MO) from wastewater under visible‐light irradiation. A heterojunction Nb6–1/CZS/g‐CN loaded with 0.01 g K7HNb6O19 showed excellent photocatalytic performance, with the MO photodegradation efficiency of 94% in 1 h and the Cr (VI) (150 mg/l) photoreduction efficiency as high as 91% in 2 hr. The main active species were deemed to be O2.‐. Additionally, the as‐prepared ternary heterojunction exhibits superior hydrogen evolution reaction (HER) rate. A heterojunction Nb6–4/CZS/g‐CN loaded with 0.5 g K7HNb6O19 exhibited the highest H2 evolution rate as high as 1777.86 μmol h?1 g?1 under visible‐light illumination, which is increased to 5.7 and 2.7 times that of bare CZS and biphase heterojunction CZS/g‐CN. These findings afford a new class of promising low‐cost photocatalyst bodying for its huge potential value in sustainable energy development and wastewater treatment.  相似文献   

17.
Photocatalytic hydrogen evolution by water splitting is highly important for the application of hydrogen energy and the replacement of fossil fuel by solar energy, which needs the development of efficient catalysts with long-term catalytic stability under light irradiation in aqueous solution. Herein, Zn0.5Cd0.5S solid solution was synthesized by a metal–organic framework-templated strategy and then loaded with MoS2 by a hydrothermal method to fabricate a MoS2/Zn0.5Cd0.5S heterojunction for photocatalytic hydrogen evolution. The composition of MoS2/Zn0.5Cd0.5S was fine-tuned to obtain the optimized 5 wt % MoS2/Zn0.5Cd0.5S heterojunction, which showed a superior hydrogen evolution rate of 23.80 mmol h−1 g−1 and steady photocatalytic stability over 25 h. The photocatalytic performance is due to the appropriate composition and the formation of an intimate interface between MoS2 and Zn0.5Cd0.5S, which endows the photocatalyst with high light-harvesting ability and effective separation of photogenerated carriers.  相似文献   

18.
Oxygen Vacancy (OVs) and carbon doping of the photocatalyst body will significantly enhance the photocatalytic efficiency. However, synchronous regulation of these two aspects is challenging. In this paper, a novel C@TiO2-x photocatalyst was designed by coupling the surface defect and doping engineering of titania, which can effectively remove rhodamine B (RhB) and has a relatively high performance with wide pH range, high photocatalytic activity and good stability. Within 90 minutes, the photocatalytic degradation rate of RhB by C@TiO2-x (94.1 % at 20 mg/L) is 28 times higher than that of pure TiO2. Free radical trapping experiments and electron spin resonance techniques reveal that superoxide radicals (⋅O2−) and photogenerated holes (h+) play key roles in the photocatalytic degradation of RhB. This study demonstrates the possibility of regulating photocatalysts to degrade pollutants in wastewater based on an integrated strategy.  相似文献   

19.
A new paratungstate-A-based organic–inorganic hybrid compound with the chemical formula of [Co(en)3]2[H2W7O24]·8H2O (en = ethylenediamine) (1) has been hydrothermally synthesized and structurally characterized by the elemental analysis, IR, TG, powder X-ray diffraction (PXRD) and single-crystal X-ray diffraction. Compound 1 crystallizes in the monoclinic space group P21/c with a = 17.216(3) Å, b = 14.986(3) Å, c = 23.088(8) Å, β = 128.151(2)°, V = 4684.2 Å3, Z = 1, R1 = 0.0484, and wR2 = 0.1087. The structure of 1 consists of the [H2W7O24]4− building blocks and [Co(en)3]2+ metal-organic cationic moieties, which are packed together via the electrostatic forces and extensive hydrogen-bonding interactions to form a three-dimensional supramolecular framework. Interestingly, compound 1 represents the first structurally-defined hybrid compound based on the metastable paratungstate-A polyoxoanions and metal–organic units. The degradation of Rhodamine-B (RhB) under UV irradiation with 1 as the heterogeneous photocatalyst has been investigated, showing a good photocatalytic property of 1 for RhB degradation.  相似文献   

20.

This present investigation focused on novel p-type bismuth ferrite (BiFeO3)/n-type tin sulfide (SnS2) heterostructure photocatalyst has been favorably attained via a facile two-step process followed by co-precipitation approach for enhances the photocatalytic activity through the degradation of Methylene Blue (MB) and Rhodamine B (RhB) organic dyes under visible-light illumination. Structural, optical, and photocatalytic behavior of the prepared BiFeO3 and BiFeO3/SnS2 photocatalysts are carefully explored. The photocatalytic efficiency of BiFeO3/SnS2 nanocatalyst was calculated to be 83%, 78% for MB and RhB, respectively, within 120 min illumination whereas the pure BiFeO3 nanoparticle was 58% and 56% for MB and RhB. This prominent enhancement of visible light photocatalytic activity can be ascribed to the separation as well as the transfer of photogenerated charge carriers, successful exploitation of visible light absorption and donates the enlarged number of photocatalytic active sites by the formation of BiFeO3/SnS2 p-n heterojunction.

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