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1.
采用硼氢化钠还原法制备了Ag负载CdMoO4光催化剂。运用X射线粉末衍射(XRD)、扫描电镜(SEM)和透射电镜(TEM)等测试手段对催化剂的组成和结构进行了表征;采用紫外-可见漫反射光谱(UV-Vis DRS)和X射线光电子能谱(XPS)等技术对催化剂的光响应和表面状态进行了分析,考察了不同Ag负载量对CdMoO4紫外光降解罗丹明B和可见光选择性氧化苯甲醇性能的影响。结果表明,与CdMoO4相比,Ag/CdMoO4具有更高的光催化活性。利用活性物种捕获实验探讨其光催化降解过程的反应机理,实验结果显示O2-·和·OH是光催化降解过程的主要活性物种。  相似文献   

2.
《中国化学快报》2022,33(11):4756-4760
Molecular oxygen (O2) is activated to reactive oxygen species (ROS) by transferring energy and carriers in the photocatalytic process, which plays an important role in environmental remediation. Herein, Cs-doped carbon nitride (CN-xCs, x = 0.2, 0.8, 1) was prepared by CsCl directly inducing the structural reconstruction of carbon nitride (CN), which had obvious molecular oxygen activation ability to promote tetracycline (TC) degradation. Besides, we explored the influence of Cs doping concentration. As a consequence, the doping concentration of Cs was an important factor affecting the activation of O2, which could cause changes in the physical and chemical structure of CN, make O enter the CN structure, form N vacancy defects and cyano groups. In addition, a proper amount of Cs doping could reduce the band gap value, increase the light absorption range, have better charge separation and transfer performance, which could remarkably promote the activation of O2. Benefiting from these advantages, CN-0.8Cs could generate a higher concentration of superoxide radicals (?O2?, 179.30 µmol/L), which was much higher than CN (6.22 µmol/L). Therefore, it exhibited excellent TC degradation photocatalytic performance, and the rate constant k of TC degradation was 0.020 min?1, which was 6.7 times the degradation rate of CN (k = 0.0030 min?1). Furthermore, the possible degradation pathways of TC were proposed based on the results of HPLC-MS.  相似文献   

3.
In this paper, to further boost the photocatalytic performance of CdMoO4, Bi3+ was successfully doped into CdMoO4 by a facile microwave hydrothermal method. The Bi-doped CdMoO4 photocatalysts prepared were characterized by Brunauer-Emmett-Teller (BET) method, X-ray diffraction (XRD), UV–Vis diffuse reflectance spectroscopy (DRS), scanning electron microscopy (SEM), energy dispersive spectrometer (EDS), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), electron spin-resonance (ESR) and surface photovoltage spectroscopy (SPS). The results exhibit that doping Bi3+ into CdMoO4 remarkably boosts the separation rate of photoinduced charge pairs and the specific surface area, decrease the crystal size, narrows the band gap of the CdMoO4 and induces the binding energy shift of Cd, all these advantageous factors result in the promoted photocatalytic performance of CdMoO4. Using rhodamine B (RhB) as model toxic pollutant, the photocatalytic activities of the photocatalysts were evaluated under a 500 W Xe lamp irradiation. When the molar ratio of Bi/Cd is 0.2%, Bi-CdMoO4 prepared displays the best photocatalytic performance, the photocatalytic performance of the 0.2% sample is more than twice of that of the reference CdMoO4.  相似文献   

4.
采用硼氢化钠还原法制备了Ag负载Cd Mo O4光催化剂。运用X射线粉末衍射(XRD)、扫描电镜(SEM)和透射电镜(TEM)等测试手段对催化剂的组成和结构进行了表征;采用紫外-可见漫反射光谱(UV-Vis DRS)和X射线光电子能谱(XPS)等技术对催化剂的光响应和表面状态进行了分析,考察了不同Ag负载量对Cd Mo O4紫外光降解罗丹明B和可见光选择性氧化苯甲醇性能的影响。结果表明,与Cd Mo O4相比,Ag/Cd Mo O4具有更高的光催化活性。利用活性物种捕获实验探讨其光催化降解过程的反应机理,实验结果显示O2-·和·OH是光催化降解过程的主要活性物种。  相似文献   

5.
《中国化学快报》2023,34(3):107535
Developing a high-quality photoelectrode for photoelectrochemical applications is still an ongoing challenge. In this study, we prepared the g-C3N4 film on the indium tin oxide (ITO) glass through conventional coating, liquid-based growth, in-situ calcination, and vapor deposition methods, respectively. These electrodes were characterized and used as photoanodes to degrade methylene blue (MB) in water. Among these methods, the in-situ calcination method was most appropriate for preparing the continuous and organized g-C3N4 film electrodes with uniform g-C3N4 coverage and strong adhesion to the ITO substrate. It also had the highest activity in the photocatalytic (PC), electrochemical (EC), and photoelectrocatalytic (PEC) degradation processes of MB. In the PEC reaction, at an applied potential of 1.0 V and a light intensity of 0.96 W/cm2, the removal rate of MB was 62.5%, which was much higher than those in the PC and EC reactions. The high degradation rate was due to the synergistic effect of PEC degradation, wherein the PC and EC reactions promote and optimize each other. In the PC reaction, MB was degraded by ?CH3 elimination, while the EC degradation pathway mainly included the conversion of sulfhydryl into sulfoxide and the opening of the central aromatic ring. Both methyl loss and aromatic ring opening occurred in the PEC reaction. Moreover, some monocyclic compounds were formed, and MB showed more complete degradation in the PEC reaction.  相似文献   

6.
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   

7.
Nanoscale anatase TiO2 single crystals were successfully synthesized using three kinds of activated carbon (AC) templates through a simple sol–gel method. The optimal photocatalyst (T‐WOAC) was obtained using wood‐based AC template. X‐ray diffraction, transmission electron microscopy and Brunauer–Emmett–Teller analyses revealed that T‐WOAC possessed a small crystallite size of 8.7 nm and a clear mesoporous structure. The photocatalytic properties of samples were then evaluated through photodegradation of crystal violet (CV). Results implied that the photocatalysts prepared using the AC templates exhibited superior photocatalytic activity to that of the original TiO2. This enhancement may be due to the small crystallite size, large specific surface area and pore volume of the catalysts prepared with ACs. T‐WOAC showed high photocatalytic activity, CV degradation of 99.01% after 120 min of irradiation and k = 0.03914 min?1, which is 3.9 times higher than that of the original TiO2 (k = 0.00994 min?1). This result can be mainly attributed to the application of WOAC with moderate specific surface area and pore volume to produce T‐WOAC. Alkaline conditions benefitted the photodegradation of CV over photocatalysts. This work proposes a possible degradation mechanism of CV and indicates that the fabricated photocatalysts can be used to effectively remove CV from aqueous solutions.  相似文献   

8.
Using a grinding method, nanocomposites of graphitic carbon nitride (g-C3N4) and magnesium aluminate (MgAl2O4) spinel were successfully synthesized for the photocatalytic degradation of methylene blue (MB) and methyl orange (MO). Variously formulated g-C3N4/MgAl2O4 nanocomposites were characterized by thermal gravimetric analysis (TGA), X-ray diffractometry (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy equipped with energy dispersive spectroscopy (SEM/EDS), transmission electron microscopy (TEM) and surface area and micropore analysis (BET surface area). The g-C3N4 powder exhibited a nanosheet structure whereas the MgAl2O4 spinel comprised agglomerated nanoparticles. The optical properties of the g-C3N4/MgAl2O4 nanocomposites were investigated by diffuse reflectance spectroscopy (DRS). As the g-C3N4 loading content increased from 0 to 30%, the optical band gap energy of the nanocomposite decreased from 3.84 to 2.86 eV, the specific surface area decreased from 153.78 to 114.45 m2/g, and the porosity decreased from 0.447 to 0.347 cm3/g. A 20%g-C3N4/MgAl2O4 nanocomposite proved to be the most effective photocatalyst and degraded MB faster and more completely than MO. The degradation rates of both MO (0.0107 min?1) and MB (0.0386 min?1) in a mixed MO-MB system were greater than the degradation rates in their single systems. The key factor that improved the photocatalytic degradation of MO was the synergistic effect whereas the synergistic effect and photosensitization were the key factors that enhanced the photocatalytic degradation of MB. The g-C3N4/MgAl2O4 nanocomposite is suitable for the photocatalytic degradation of mixed dyes because its point of zero charge is neutral and it is stable and recyclable.  相似文献   

9.
采用机械球磨法制备Y~(3+)修饰TiO_2光催化剂,利用紫外-可见漫反射光谱(UV-Vis DRS)、X射线光电子能谱(XPS)、X射线粉末衍射(XRD)、扫描电镜(SEM)等对其进行表征,在紫外光下,以亚甲基蓝(MB)为去除物来考察催化剂活性并优化球磨工艺。将最佳条件下制得的Y~(3+)/TiO_2光催化剂负载于不同半径的塑料浮球上,分别在紫外光和模拟太阳光照射下处理海水养虾废水,通过CODCr(chemical oxygen demand)及三维荧光观察有机物含量变化。结果表明,当Y~(3+)的物质的量分数为2%,球磨时间4 h,球料质量比4∶1,转速为500 r·min~(-1)时,MB光催化降解反应速率常数可达0.111 3 min~(-1),是纯TiO 2的4.2倍。由UV-Vis DRS、XPS、N_2吸附-脱附、XRD、SEM等表征结果显示,2%Y~(3+)/TiO_2样品的禁带宽度降低至3.05 eV,光吸收发生红移,并产生可见光响应,表面吸附氧含量明显增加,比表面积增大到104 m~2·g~(-1)。采用纯TiO_2及2%Y~(3+)/TiO_2为光催化剂处理养虾废水,在可见光和紫外光下CODCr的去除率分别为14.7%和18.8%、26.9%和37.5%。考察3种直径分别为1、2、3 cm负载Y~(3+)/TiO_2浮球的光催化效果,显示直径为2 cm浮球效果最佳,CODCr去除率可达38.5%。  相似文献   

10.

This work reports an innovative, effortless and inexpensive method for the preparation of ZnO nanoparticles by green approach using leaf extract of Piper betleas a reducing-stabilizing negotiator. The prepared ZnO NPs were characterized through XRD, FTIR, UV–Visible spectroscopy, and EDX etc. The band gap energy of the sample was estimated as 3.41 eV which is larger than the bulk ZnO (Eg?=?3.37 eV). The observed blue shift is attributed to the quantum confinement of excitons. FTIR analysis showed the presence of alkaloids, flavonoids, polyphenols, and terpenoid. TEM analysis showed that each nanoparticle comprised of 1 to 2 nano-crystallites. Photocatalytic activity results revealed that ZnO-NPs prepared through green synthesis route were found to be efficient in the degradation of toxic reactive red dye with degradation efficiency of 96.4% having high photodegradation rate-constant of 1.6?×?10–2 min?1. As an antimicrobial agent, the ZnO NPs are effective against both gram-positive (Bacillus subtilis) and negative bacteria (Escherichia coli), with the zones of clearance as 16.4 and 14.3 mm, respectively. Therefore, present research signifies an effective approach to utilize as-prepared ZnO NPs as efficient photocatalysts as well as antimicrobial agent.

  相似文献   

11.
Calcium stannate (CaSnO3) was successfully synthesized in the solutions containing different surfactants by cyclic microwave and calcination combination. Phase, morphology and vibration mode were characterized by X-ray diffraction, field emission scanning electron microscopy and Fourier transform infrared spectroscopy. Growth mechanism of the products was also explained according to the analytical results. Their photocatalytic activities were tested through methylene blue (MB) degradation induced by UV radiation. In the MB solution with pH 6, the S-CTAB product showed the highest decolorization efficiency of 89.1% and the highest rate constant of 4.374?×?10?3 min?1.  相似文献   

12.
以水热法制备的20% g-C3N4/TiO2(20%为质量分数)为基,将其与不同质量分数的氧化石墨烯(GO)复合制备出可见光催化性能优良的GO/TiO2-g-C3N4三元复合材料。利用X射线衍射(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)、光致荧光光谱(PL)、瞬态光电流响应等分析测试手段对样品的结构、形貌和光电性能进行表征。研究了不同质量分数GO的加入对GO/TiO2-g-C3N4在可见光下降解亚甲基蓝(MB)溶液的影响。结果表明: g-C3N4/TiO2与GO复合后,锐钛矿相TiO2颗粒形成小团簇附着在g-C3N4和GO片层表面,且当GO含量为15%时,TiO2形成的团簇最小,对可见光的吸收最多且光生电子-空穴对的复合率最低。可见光照射下,15% GO/TiO2-g-C3N4复合材料对MB的降解率在3 h内可达98.4%,且其降解速率常数(0.022 4 min-1)分别是纯TiO2(0.001 5 min-1)和g-C3N4/TiO2(0.002 5 min-1)的15倍和9倍。  相似文献   

13.
Recently, graphitic carbon nitride (CN) has been widely investigated for solar energy conversion through water splitting, but its low photocatalytic activity needs to be further improved and optimized. Herein, S/K co‐doped CN photocatalysts have been fabricated by condensation of thiourea and dithiooxamide followed by post‐treatment in molten salt. As evidenced by XRD patterns and UV–vis DRS plots, the engineering crystalline and electronic structure of all as‐prepared samples have been explored through tailoring the mass ratio of thiourea and dithiooxamide as well as ratio of molten salt/the precursor. After optimization, the as‐prepared S/K co‐doped CN photocatalysts with needle‐like nanorods structure exhibit excellent hydrogen evolution rate of 1962.10 μmol?1 g?1 h?1. While its photocatalytic activity is lower than that of pure CN by molten salt treatment (K‐doped CN) (2066.40 μmol?1 g?1 h?1), which results from that the K content of S/K co‐doped CN photocatalyst is lower than that of K‐doped CN. Moreover, compared with K‐doped CN, S/K co‐doped CN photocatalyst possesses higher photocatalytic performance when irradiated by a light source (λ > 520 nm). This might be ascribed to the fact that the introduction of sulfur can expand light absorption region (λ > 520 nm), whereas K cannot improve light absorption of CN in this wavelength region. Furthermore, DFT calculation reveals that both S and K atoms can offer more electrons to band gap, leading to the formation of metallic‐character band structure. In addition, K atom can intercalate in the interlayer of CN and bridge the adjacent two layers, leading to the formation of charge delivery channels. These results demonstrate that S/K co‐doped CN photocatalysts facilitate the separation and transport of photogenerated charge carries, resulting in the efficient photocatalytic activity for hydrogen evolution. Besides, a competition between sulfur and potassium atom during the synthesis process is also discussed in details.  相似文献   

14.
《印度化学会志》2021,98(10):100140
In recent years, the transition-metal tungstate materials with formula MWO4 have attracted much attention in photocatalytic environmental purification due to their interesting structural and optical properties. Among the others, manganese tungstate (MnWO4) has attracted particular attention because of its appropriate bandgap energy (2.67 ​eV) with tunable optical and electrical properties, chemical stability, and low cost which makes a suitable photocatalyst. Nevertheless, the manganese tungstate (MnWO4) based materials are less explored as visible light responsive photocatalysts for wastewater purification. Hence, both parent and N-doped MnWO4 are synthesized by a hydrothermal method with different nitrogen contents (5, 10, and 15 ​mol%). The as-prepared photocatalysts were characterized by XRD, SEM-EDS, TEM-SAED, FT-IR, UV–Vis DRS, XPS and PL techniques. The photocatalytic activities of the synthesized samples were evaluated by degradation of methylene blue (MB) dye under the visible light irradiation. All the N-doped MnWO4 samples exhibited enhanced visible-light photocatalytic activity compared to the parent MnWO4, and the optimal dopant amount of nitrogen was 15 mol% for the best photocatalytic activity. The active species generated during the process of MB degradation are investigated by scavenging experiments. Further, the reusability of the 15 ​mol% N-doped MnWO4 photocatalyst was examined in three consecutive catalytic runs.  相似文献   

15.
16.
High aspect ratio cobalt doped ZnO nanowires showing strong photocatalytic activity and moderate ferromagnetic behaviour were successfully synthesized using a solvothermal method and characterized by scanning electron microscopy (SEM), X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), X-ray absorption spectroscopy (XAS), vibrating sample magnetometry (VSM) and UV–visible absorption spectroscopy. The photocatalytic activities evaluated for visible light driven degradation of an aqueous methylene orange (MO) solution were higher than for Co doped ZnO nanoparticles at the same doping level and synthesized by the same synthesis route. The rate constant for MO visible light photocatalytic degradation was 1.9·10−3 min−1 in case of nanoparticles and 4.2·10−3 min−1 in case of nanowires. We observe strongly enhanced visible light photocatalytic activity for moderate Co doping levels, with an optimum at a composition of Zn0.95Co0.05O. The enhanced photocatalytic activities of Co doped ZnO nanowires were attributed to the combined effects of enhanced visible light absorption at the Co sites in ZnO nanowires, and improved separation efficiency of photogenerated charge carriers at optimal Co doping.  相似文献   

17.
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   

18.
Bi2S3/g-C3N4 (BSCN) samples with different mass ratios of CN to BS were prepared by a facile and practicable hydrothermal method with 2D g-C3N4 nanosheets (CN). The microscopic morphology and structure of pure CN, BS and BSCN were measured by multiple testing methods. Analysis results show that the BSCN was prepared successfully, and the Bi2S3 nanoparticles closely and uniformly adhered to the surface of CN with sheet-like structure. The introduction of Bi2S3 did not change the structure of the CN. The results of the ultraviolet–visible spectroscopic analysis, photoluminescence spectra and electrochemical performance indicated that BSCN showed superior visible-light response compared with CN, and the separation and transfer efficiency of photogenerated carriers was significantly improved. With the decrease of mass ratio of CN/BS, the photocatalytic activity of BSCN initially increased and then decreased for 20 ppm of Rhodamine B solution (RhB), and the Bi2S3/g-C3N4-B with a mass ratio of 8:1 for CN to BS showed optimal photocatalytic performance (98.98%). Furthermore, the Bi2S3/g-C3N4-B exhibited apparent degradation effects (1.021 x10-2, 0.879 x10-2 and 0.793 x10-2 min?1) to three kinds of antibiotics (tetracycline, ciprofloxacin, and oxytetracycline). The BSCN samples still maintained higher degradation efficiency after five cycles of degradation to tetracycline. The capture experiments and the electron spin resonance (ESR) spectra analysis indicated that the h+ and ·O2? played a major role, and ·OH played secondary role during the photocatalytic reaction.  相似文献   

19.
《Comptes Rendus Chimie》2014,17(7-8):818-823
A series of W-modified TiO2 (W–TiO2) photocatalysts were synthesized by a simple sol–gel method. The new photocatalysts were characterized by X-ray diffraction (XRD), X-ray fluorescence (XRF), scanning electron microscopy (SEM), transmission electron microscopy (TEM), UV–vis-diffuse reflectance spectroscopy (DRS), and Brunauer, Emmett and Teller (BET) surface area analyzer. The photoactivity of the W–TiO2 photocatalysts was evaluated by the photocatalytic oxidation of Congo red (CR) dye. It was found that the average size of the prepared photocatalysts is 10 nm. Moreover, they have high surface areas (∼ 216 m2 g−1) and their light-absorption extends to the visible region compared to pure TiO2. The effects of W-loading and of the calcination temperature of the prepared photocatalysts on their photocatalytic activity were also studied. The obtained results show that the W0.5–TiO2 photocatalyst calcined at 350 °C is much highly photoactive than non-doped or highly doped TiO2. The enhanced photocatalytic activity of the weakly doped TiO2 may be attributed to the increase in the charge separation efficiency and the presence of surface acidity on the W0.5–TiO2 photocatalyst.  相似文献   

20.
Novel NiO/Cd/g-C3N4 photocatalysts were synthesized using a green and straightforward microwave-assisted method and characterized by X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), the Brunauer–Emmett–Teller (BET) method, transmission electron microscopy (TEM), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), and ultraviolet–visible spectroscopy (UV–Vis). The ternary NiO/Cd/g-C3N4 nanocomposites were evaluated for the degradation of methylene blue (MB) at room temperature under the visible light irradiation. Experimental results revealed that the weight percent of cadmium had a remarkable effect on the photodegradation efficiency. The NiO/Cd/g-C3N4 (0.1%) sample exhibited superior activity in the degradation reaction. The activity of this nanocomposite was about 4.5 and 3.25 fold higher than those of the pure g-C3N4 and NiO/g-C3N4 samples in the degradation of MB, respectively. The enhanced photocatalytic activity was attributed to the low energy gap, increased absorption capacity of the visible light, and efficient suppression of the recombination of photogenerated electron-hole pairs. A detailed photocatalytic mechanism over the nanocomposite of NiO/Cd/g-C3N4 (0.1%) was proposed with superoxide radical anion O2 as the main reactive species. The stability of the nanocomposite was confirmed after four consecutive runs as well.  相似文献   

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