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1.
A novel ZnCo2O4/Bi2O3 heterojunction photocatalyst was prepared via balling method. The enhanced photocatalytic activity is mainly attributed to the broad photoabsorption and low recombination rate of photogenerated electron-hole pairs, which is driven by the photogenerated potential difference formed at the ZnCo2O4/Bi2O3 heterojunction interface.  相似文献   

2.
Spinel structure nickel ferrite (NiFe2O4) doped graphitic carbon nitride (g-C3N4) photocatalyst NiFe2O4/g-C3N4 was synthesized by the coprecipitation route to enhance the photocatalytic activity for the visible-light driven degradation of methyl orange. The NiFe2O4 doping content is responsible for the microstructure and photocatalytic activity of NiFe2O4/g-C3N4 samples. Compared with pure NiFe2O4 and g-C3N4, the 2-NiFe2O4/g-C3N4 composite with NiFe2O4 doping of 2.0 wt% exhibited excellent photocatalytic activity and superior stability after five runs for degrading methyl orange under visible light irradiation. The catalytic activity of 2-NiFe2O4/g-C3N4 sample produced using the coprecipitation route was higher than those of conventional 2-NiFe2O4/g-C3N4 bulks prepared by the impregnation approach. The prepared samples for the photocatalytic degradation of methyl orange followed pseudo-first-order reaction kinetics. It’s ascribed to the synergistic effect between NiFe2O4 and g-C3N4, which can inhibit the recombination of photoexcited electron-hole pairs, accelerate photoproduced charges separation, and enhance the visible light absorption.  相似文献   

3.
A very simple and controllable approach was proposed to synthesize novel Fe(OH)_3/TiO_2 nanoparticles.Compared with neat TiO2,the Fe(OH)_3/TiO_2 increased the rate of the photocatalytic degradation of methyl orange at pH 6.0 by more than five times, showing photocatalytic activity as excellent as P25.This enhancing effect is mainly attributed to the ferric hydroxide deposits as the electron scavenger and the enriched surface hydroxyl groups.  相似文献   

4.
《中国化学快报》2021,32(9):2787-2791
A novel carbon-rich g-C3N4 nanosheets with large surface area was prepared by facile thermal polymerization method using urea and 1,3,5-cyclohexanetriol. Plenty of carbon-rich functional groups were introduced into the surface layers of g-C3N4, which constructed the built-in electric field (BIEF) and resulted in improved charge separation; therefore, the carbon-rich g-C3N4 displayed superior photocatalytic activity for amoxicillin degradation under solar light. The contaminant degradation mechanism was proposed based on radical quenching experiments, intermediates analysis and density functional theory (DFT) calculation. Moreover, the reusing experiments showed the high stability of the material, and the amoxicillin degradation under various water matrix parameters indicated its high applicability on pollutants treatment, all of which demonstrated its high engineering application potentials.  相似文献   

5.
Ag3PO4 is widely used in the field of photocatalysis because of its unique activity. However, photocorrosion limits its practical application. Therefore, it is very urgent to find a solution to improve the light corrosion resistance of Ag3PO4. Herein, the Z-scheme WO3(H2O)0.333/Ag3PO4 composites are successfully prepared through microwave hydrothermal and simple stirring. The WO3(H2O)0.333/Ag3PO4 composites are characterized by X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy and UV-Vis spectroscopy. In the degradation of organic pollutants, WO3(H2O)0.333/Ag3PO4 composites exhibit excellent performance under visible light. This is mainly attributed to the synergy of WO3(H2O)0.333 and Ag3PO4. Especially, the photocatalytic activity of 15%WO3(H2O)0.333/Ag3PO4 is the highest, and the methylene blue can be completely degraded in 4 min. In addition, the stability of the composites is also greatly enhanced. After five cycles of testing, the photocatalytic activity of 15%WO3(H2O)0.333/Ag3PO4 is not obviously decreased. However, the degradation efficiency of Ag3PO4 was only 20.2%. This indicates that adding WO3(H2O)0.333 can significantly improve the photoetching resistance of Ag3PO4. Finally, Z-scheme photocatalytic mechanism is investigated.  相似文献   

6.
Due to unique properties, KCa2Nb3O10 compound has received great attention worldwide. High-temperature solid-state reaction is the common route for the synthesis of this compound. In order to propose a new low-temperature method (i.e. hydrothermal synthesis), which could improve the final properties of KCa2Nb3O10, this study has been planned and performed. The preliminary experiments in KOH-Nb2O5 and Ca(OH)2-Nb2O5 systems revealed that KCa2Nb3O10 could be hydrothermally synthesized from a KOH-Ca(OH)2-Nb2O5 system using an alkaline condition (i.e. 5 M < KOH <10 M). However, the experimental results showed that the product only consisted of KNbO3 and Ca2Nb2O7 phases. To initiate the reaction between KNbO3 and Ca2Nb2O7, the obtained KNbO3-Ca2Nb2O7 mixture was heat-treated in an air atmosphere. The results showed that KCa2Nb3O10, with a high crystallinity and good purity, has been successfully obtained at 800 °C. This temperature is the lowest temperature, reported for the synthesis of KCa2Nb3O10 compound so far. The SEM investigations revealed that the obtained KCa2Nb3O10 powder has plate-like morphology due to its layered structure.  相似文献   

7.
金属磷酸盐材料在吸附、离子交换、离子传导和催化剂方面有潜在的应用前景[1~5]. 近年来, 通过水热反应合成了一些A-V-P-O化合物. 在这些化合物中, A一般为碱金属或有机阳离子, 如层状结构的[H2N(C4H8)2NH2][(VO)4(OH)4(PO4)2][6] 和[H2N(C2H4)3NH2][(VO)8(HPO4)3(PO4)4*(OH)2]*2H2O[6], 一维链状结构的 [H2NCH2CH2NH3(VO)(PO4)][7], 手性双螺旋结构的 [(CH3)2NH2]K4[(VO)10(H2O)2(OH)4(PO4)7]*H2O[8]以及具有三维骨架结构的化合物 [H3N(CH2)3NH3K(VO)3(PO4)3][9], [H3N(CH2)3NH3]2[V(H2O)2(VO)6(OH)2(HPO4)3(PO4)5]*3H2O[10]和[H3N(CH2)2NH3][(VO)3(H2O)2(PO4)2(HPO4)4][11].  相似文献   

8.
In this work, Fe2O3 nanoparticles, abbreviated as OL and OS, were facilely synthesized by the combustion procedure using L-lysine and L-serine as organic fuels, respectively. Also, the OL and OS samples were identified using different instruments such as Raman spectrometer, FT-IR spectrophotometer, UV–Vis spectrophotometer, XRD, HR-TEM, BET surface area, and FE-SEM. The XRD confirmed that the mean grain size of OL and OS samples is 42.23 and 33.16 nm, respectively. The HR-TEM images confirmed that irregular, hexagonal, and spherical shapes, have an average diameter of 39.13 and 34.28 nm, were observed in the OL and OS samples, respectively. The BET surface area of the OL and OS samples is 16.20 and 28.34 m2/g, respectively. Additionally, the OL and OS samples were accomplished for the photocatalytic degradation of methylene blue dye in the absence and presence of hydrogen peroxide. The % degradation of 45 mL of 25 mg/L of methylene blue dye in the case of using OL and OS samples in the absence of hydrogen peroxide is 55.23 and 63.64 % after 120 min, respectively. Also, in the presence of hydrogen peroxide, the % degradation in the case of using OL and OS samples is 100 % after 35 and 25 min, respectively.  相似文献   

9.
Fabrication of heterojunction with specialized geometry shape could improve the photodegradation efficiency of catalysts more efficiently based on the synergistic effect of components. Herein, the BiVO4/ZnCr-LDH type-II heterojunction was successfully synthesized by the growth of two-dimensional (2D) ZnCr-LDH on 2D BiVO4, forming a unique three-dimensional (3D) hierarchical structure. The 3D hierarchical BiVO4/ZnCr-LDH type-II heterojunction with intimate 2D/2D heterointerfaces enlarges the interfacial contact areas and shortens the transfer distance of carriers simultaneously, which could promote the separation and transfer of photoinduced carriers and prolong the lifetime of carriers. Additionally, the 3D structure could enhance the photon utilization efficiency caused by the multiple reflections of incident light, and provide more active sites to promote the adsorption of pollutants. Therefore, the visible light catalytic performance of the optimal heterostructure for the removal of tetracycline hydrochloride is 3.47 times and 22.43 times higher than that of BiVO4 and ZnCr-LDH, respectively. Superoxide radical (O2?) is confirmed as the primary active species, whereas hole (h+) is the secondary active species in the photodegradation process. This work provides a facile strategy to enhance the visible light catalytic behavior of BiVO4 through the fabrication of 3D hierarchical architecture heterojunction for the removal of organic pollutant.  相似文献   

10.
《印度化学会志》2021,98(12):100239
Highly photosensitive novel nanostructure CoCr2O4@GeO2@ZnO core-shell UV–Visible light driven photocatalyst have been fabricated by sol-gel method. The double coating of GeO2 and ZnO on CoCr2O4 nanoparticles could intensely stabilize the CoCr2O4 in aqueous solution and avoid their oxidation. The synthesized CoCr2O4, CoCr2O4@GeO2, and CoCr2O4@GeO2@ZnO nanostructures were characterized by several techniques including FT-IR, XRD, UV-DRS FE-SEM, EDS, HR-TEM and BET analysis. The potential application of CoCr2O4@GeO2@ZnO is examined for photocatalytic degradation of Basic Fuchsin dye in aqueous heterogeneous suspension. The detailed degradation pathway has been established by using LC-MS analysis and by a careful identification of intermediate products. The result suggest that CoCr2O4@GeO2@ZnO photocatalysis may be envisaged as a method for treatment of diluted waste water in textile industries. In the present study, the degradation yield for Basic Fuchsin dye 100% within 30 ​min using core-shell CoCr2O4@GeO2@ZnO nanostructure material.  相似文献   

11.
12.
Sokolov  M. N.  Dybtsev  D. N.  Virovets  A. V.  Clegg  W.  Fedin  V. P. 《Russian Chemical Bulletin》2001,50(7):1144-1147
The supramolecular complex {[Cl3InW3S4(H2O)9]2(C36H36N24O12)}Cl4·28H2O was prepared by mixing solutions of [Cl3InW3S4(H2O)9]2+ and cucurbituril in hydrochloric acid. The molecular and crystal structure of the resulting complex was established by X-ray diffraction analysis.  相似文献   

13.
《中国化学快报》2020,31(10):2784-2788
Efficient generation of singlet oxygen (1O2) by an excitonic energy transfer process is highly desired on a semiconductor photocatalyst for selective oxidation of methyl phenyl sulfide (MPS). Herein, it is demonstrated that a large amount of 1O2 is produced on pristine graphitic carbon nitride (CN) nanosheet compared with bismuth oxybromide (BiOBr) and commercial P25 titanium dioxide (TiO2). This leads to a certain photoactivity of CN for MPS oxidation. The observed ∼77% selectivity for CN depends on the competitive results of excitonic energy transfer for 1O2 formation and charge carrier separation for superoxide radical (O2) production, which are based on the phosphorescence spectra and electron paramagnetic resonance signals, respectively. Moreover, ultrathin CN nanosheets are synthesized by thermal treatment with the cyanuric acid-melamine hydrogen bonded aggregates as precursors. It is confirmed that the amount of produced 1O2 could be increased by decreasing the thickness of resultant CN nanosheets. The optimized ultrathin CN nanosheet (∼4 nm) exhibits excellent photoactivity with high selectivity (∼99%). It is suggested that the excitonic energy transfer for 1O2 formation is close related to the intrinsic exciton binding energy and the two-dimensional quantum confinement effect. This work establishes a basic mechanistic understanding on the excitonic processes in CN, and develops a feasible route to design CN-based photocatalysts for efficient 1O2 generation.  相似文献   

14.
近年来,化石燃料燃烧导致的环境污染问题和能源危机越来越严重.在众多解决方案中,光催化产氢由于其可持续性以及无污染等特点而受到广泛关注.然而,由于许多半导体光催化剂性能不理想,光催化水分解研究进程缓慢.本研究采用水热法成功制备了梯型Pg-C3N4/Zn0.2Cd0.8S-DETA复合材料用于光催化产氢.DETA(二亚乙基三胺)作为一种有机分子插入在Zn0.2Cd0.8S的层中构成有机-无机杂化材料.采用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-可见光漫反射光谱(UV-vis)以及光电流研究了所制备样品的结构、形貌、元素组成以及光电特征,并提出了可能的光催化机制.XRD和XPS结果表明Pg-C3N4和Zn0.2Cd0.8S-DETA复合在一起而不是机械混合.通过TEM可以看出Pg-C3N4是一种带有很多孔洞的纳米片,而Zn0.2Cd0.8S-DETA类似于纳米花瓣,在Pg-C3N4/Zn0.2Cd0.8S-DETA复合材料中Pg-C3N4表面充满了Zn0.2Cd0.8S-DETA纳米花瓣.经过元素分析得知所合成的复合材料没有杂质元素.UV-vis表明Pg-C3N4和Zn0.2Cd0.8S-DETA具有良好的吸收带边以及带隙,分别为2.83 eV和2.48 eV.光电流和PL显示15%Pg-C3N4/Zn0.2Cd0.8S-DETA具有很高的载流子分离及传输效率.光催化性能测试显示15%Pg-C3N4/Zn0.2Cd0.8S-DETA具有很好的产氢活性,为6.69 mmol g^-1 h^-1,分别是Pg-C3N4和Zn0.2Cd0.8S-DETA的16.73和1.44倍.在经过七次循环实验后15%Pg-C3N4/Zn0.2Cd0.8S-DETA仍保持很优异的活性,说明它具有很好的稳定性.通过高分辨XPS中各元素结合能的变化可以看出构成异质结之后电子的流向,从而看出光催化可能的机制为梯形.光照射之后,Pg-C3N4和Zn0.2Cd0.8S-DETA中产生电子-空穴对,电子迁移到导带并在价带留下空穴.当Pg-C3N4与Zn0.2Cd0.8S-DETA复合之后,在它们的接触处会形成内部电场,Zn0.2Cd0.8S-DETA导带上的电子和Pg-C3N4价带上的空穴会在内部电场作用下复合.Zn0.2Cd0.8S-DETA价带上的空穴和Pg-C3N4上的电子分别参与氧化还原反应.梯形机制促使电子和空穴在空间上分离,从而具有强氧化还原性.梯形异质结的形成加快了15%Pg-C3N4/Zn0.2Cd0.8S-DETA复合材料中电子-空穴对的分离效率,并减少了电子-空穴对的复合,从而使其具有很优异的光催化性能和稳定性.  相似文献   

15.
石墨相氮化碳(g-C_3N_4)具有独特的二维层状结构和合适的能带结构,因而在可见光催化领域广受关注.尤其是在可见光去除环境污染物领域,得到了较为充分的研究与应用.然而g-C_3N_4去除环境污机理的反应机理尚不明确.因此,本文采用理论计算与实验高度结合的研究方法,以光催化NO去除为例,深入阐述了光照下g-C_3N_4表面活性氧物种(ROS)的生成及转化过程,及其介导下的NO光催化氧化机理.X射线衍射结果表明,g-C_3N_4是三嗪环层内聚合后层层堆叠而成,并由红外光谱确定了其表面的官能团类型.该结构经扫描电镜和透射电镜得到了进一步的验证.采用光致激发谱和紫外可见漫反射光谱等实验表征与密度泛函理论计算结合的光电性质分析,我们发现,g-C_3N_4在可见光下具有一定的响应,这为其在光催化去除NO中奠定了基础.同时,其价带位置过高,无法自行产生氧化性较强的羟基自由基(.OH).电子自旋共振技术结果表明g-C_3N_4在光照下能捕获到·O_2~-和·OH两种活性自由基.采用反应路径计算发现,·OH是由·O_2~-在导带上逐步得到电子被还原而生成,其中的速率控制步骤是H_2O_2的解离.因此,促进O_2分子的吸附和活化和克服H_2O_2解离的反应活化能是产生·OH和提升g-C_3N_4光催化氧化活性的关键.采用原位红外光谱技术对g-C_3N_4上NO的氧化去除过程进行了表征,发现其主要中间产物为NO_2,主要终产物为NO_2~-和NO_3~-,采用反应路径计算对该反应过程进行了理论模拟,发现在·O_2~-介导下,最高反应活化能为0.66 eV,而在·OH介导下,该活化能降低至0.46 eV,表明·OH的氧化性要明显强于·O_2~-.总之,本文采用一种可行的、高度结合的实验与计算手段研究了g-C_3N_4上ROS的生成及转化过程及其对NO去除的反应历程,在原子尺度揭示了该反应的机理,加深了对ROS在光催化环境污染物降解过程中作用的理解.  相似文献   

16.
电荷分离及转移是影响光催化效率的重要因素之一.本文采用简易的水热焙烧法,设计并构筑了Bi2Mo3O12@Bi2O2CO3(BMO@BOC)异质结,促进了光生载流子的分离与迁移,并优化了异质结构中的BMO与BOC的组分比例,其中BMO@BOC-1样品展现了最高的光催化脱除NO效率(~35%),且具有优异的循环稳定性.SEM与TEM结果表明,BMO@BOC-1样品是由超薄纳米片构成,可以提供丰富的反应活性位点,从而促进光催化反应的发生.HRTEM,XRD及Raman充分证明已成功合成不同组分比例的BMO@BOC异质结.同时, Raman与XPS结果表明, BMO@BOC异质结由Bi, O,C及Mo组成, XPS图谱中拟合峰位置的偏移是由异质结组分不同所致.值得注意的是, UV-visDRS结果表明,BMO@BOC-4具有最好的光谱吸收性能,但它与BMO@BOC-2和BMO@BOC-1样品的吸收带边相近,而PL结果则表明BMO@BOC-1具有更好的电荷分离性能,以及合适的组分比例,在一定程度上可以促进光吸收,并能最大限度的促进光生载流子的分离.BMO@BOC-1样品的ESR测试结果说明,·OH与·O2-的含量随着光照时间的延长而增加,证实了它们是光催化NO氧化的活性中间物种.另外,光催反应机制的研究在高效光催化剂的研发及其商业化应用中具有深远意义.本文还利用原位红外实时动态监测手段,采用"连续流测试法"与"间歇流测试法"直观动态地研究了BMO@BOC异质结催化剂表面光催化NO脱除反应过程.结果表明,在开灯前的吸附阶段于催化剂表面形成了NO-, NO2-以及NO2等中间产物,开灯后的氧化阶段出现终产物(NO3-).进一步深入分析,中间产物NO-和NO2-在氧化阶段会被氧化活性物种进一步氧化成NO3-,而中间产物NO2可能作为一种毒副产物影响NO的完全氧化.综上所述,本文将为理解NO氧化过程提供直观且动态的研究方法,对光催化技术的发展具有重要的指导意义.  相似文献   

17.
A novel compound, [HN(C2H4)3N][(VO)2(HPO3)2(OH)(H2O)]·H2O, was hydrothermally synthesized and characterized by single crystal X-ray diffraction. This compound crystallizes in the monoclinic system with the space group C2/c and cell parameters a=11.0753(3) Å, b=17.8265(6) Å, c=16.5229(5) Å, and β=92.362(2)°. The structure of the compound consists of vanadium phosphite layers which are built up from the infinite one-dimensional chains of [(VO)(H2O)(HPO3)2]2− of octahedral VO5(H2O) and pseudo pyramidal [HPO3], and bridging binuclear fragments of [VO(OH)]2. Thermogravimetric analysis and magnetic susceptibility data for this compound are given.  相似文献   

18.
In this study, novel ternary Fe2O3/ZnO/ZnFe2O4 (ZFO) composites were successfully prepared through a simple hydrothermal reaction with subsequent thermal treatment. The as-prepared products were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET) analysis, Barrett-Joyner-Halenda (BJH) measurement, and UV–vis diffuse reflectance spectroscopy (UV–vis DRS). The photocatalytic degradation of rhodamine B (Rh B) under visible light irradiation indicated that the ZFO composites calcined at 500 °C has the best photocatalytic activity (the photocatalytic degradation efficiency can reach up to 95.7% within 60 min) and can maintain a stable photocatalytic degradation efficiency for at least three cycles. In addition, the photocatalytic activity of ZFO composites toward dye decomposition follows the order cationic Rh B > anionic methyl orange. Finally, using different scavengers, superoxide and hydroxyl radicals were identified as the primary active species during the degradation reaction of Rh B.  相似文献   

19.
液相法合成锂离子电池正极材料Li_(1+x)Mn_2O_4   总被引:11,自引:0,他引:11  
采用柠檬酸络合和溶液浸渍两种方法制备Li1+xMn2 O4正极材料 ,用XRD和BET测试了材料晶体结构和比表面积 ,考察焙烧温度、Li/Mn比、起始原料对产物结构和电化学性能的影响 ,结果表明 ,焙烧温度与Li/Mn比是影响材料电化学性能的关键因素 ,确定了制备Li1+xMn2 O4材料最佳条件为 0≤x≤ 0 .0 5 ,焙烧温度 75 0°C ,所得电池材料首次充放电容量达到 1 2 0mAh/g .循环 5 0次后 ,其充放电容量为 1 1 5mAh/g .  相似文献   

20.
刘超  封越  韩字童  孙耀  王晓秋  张勤芳  邹志刚 《催化学报》2021,42(1):164-174,后插28-后插31
随着人口增长和全球工业化进程加快,人们饱受环境污染和能源短缺问题的困扰.半导体光催化技术作为一种高效、可持续、环境友好、有潜力的新技术,在环境净化和能源开发方面有着广阔的应用前景.到目前为止,人们已开发出多种半导体光催化剂,并广泛应用于污染物降解、氢气制备和二氧化碳还原等领域.其中,化合物K4Nb6O17具有典型的层状结构、合适的电子能带结构、结构易改性以及良好的电荷传输性能等特点,在光催化领域得到了广泛研究.然而,单纯K4Nb6O17仍存在光响应范围窄、光生载流子复合率高等问题,限制了K4Nb6O17的进一步应用.因此,需要对K4Nb6O17进行改性,拓宽其光吸收范围,提高其光生载流子分离效率,从而提高其光催化活性.本研究通过简单焙烧法制备Z型N-掺杂K4Nb6O17/g-C3N4(KCN)异质结光催化剂,其中石墨相氮化碳(g-C3N4)在复合材料中质量比约为50%.层状K4Nb6O17层板的电子结构通过N掺杂进行调控,拓宽其光响应范围,使其具有可见光响应;同时,形成的g-C3N4位于N-掺杂K4Nb6O17的外层以及内层空间,在这两种组分之间形成异质结,有利于提高光生载流子的分离效率.荧光光谱、时间分辨荧光光谱和光电化学测试表明,N掺杂和异质结的形成有利于增强光生电子-空穴对的传输和分离效率.通过在可见光照射下降解罗丹明B(RhB)和产氢来评估材料的光催化性能.相比g-C3N4(8.24μmol/h)和Me-K4Nb6O17(~1.30μmol/h),KCN复合材料光催化产氢效率(~16.91μmol/h)得到了极大提高,并显示出极好的光催化产氢稳定性能.对于光催化降解RhB体系,KCN复合材料也显示出较好的光催化活性和稳定性,并能很好地将RhB矿化.鉴于KCN复合材料具有较小的比表面积(9.9 m^2/g)且无孔结构,认为比表面积对光催化活性影响较小.因此,与单组分相比,KCN复合材料光催化产氢和RhB降解活性都得到了极大提高,活性的增强主要归功于N掺杂和异质结形成的协同效应,其中N掺杂可以拓宽光捕获能力,异质结形成可提高电荷载流子的分离效率.电子自旋共振(ESR)谱表明,在KCN降解RhB体系中,超氧自由基(·O2^?)、羟基自由基(·OH)和空穴(h^+)作为主要活性物质都参与了反应.结合实验结果可以推测KCN复合材料满足了Z型光催化体系,该体系具有高效的光生载流子分离效率和较高的氧化还原能力.  相似文献   

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