CuxZn1-xS/RGO复合材料的制备及其光催化降解环丙沙星性能研究
Preparation and performance of CuxZn1-xS/RGO composite for photocatalytic degradation of CIP
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摘要: 通过一步水热法制备了光催化剂CuxZn1-xS/RGO,实现了CuxZn1-xS纳米颗粒的可控生长和氧化石墨烯(GO)还原的同步进行,并将所制备的CuxZn1-xS/RGO用于环丙沙星(CIP)的催化降解研究.采用X-射线衍射(XRD)、电感耦合等离子体-原子发射光谱仪(ICP-AES)、傅立叶变换红外光谱(FTIR)、紫外可见漫反射光谱(UV-Vis)、电子显微镜(SEM)和透射电子显微镜(TEM)对复合物的组成形貌进行表征.结果表明,球状的CuxZn1-xS颗粒成功负载在石墨烯表面.Cu2+的掺杂增强了CuxZn1-xS/RGO光催化剂在可见光范围的响应,石墨烯的引入抑制了CuxZn1-xS纳米颗粒的团聚,提高了光催化性能.此外,Cu0.1Zn0.9S/RGO10对CIP的降解速率分别是ZnS、Cu0.1Zn0.9S的8倍和4.4倍.Abstract: A facile approach to prepare CuxZn1-xS/RGO photocatalyst was developed via a one-step hydrothermal synthesis. Formation of CuxZn1-xS nanoparticles and the reduction of graphene oxide (GO) were achieved simultaneously in the synthesis process. The degradation of ciprofloxacin (CIP) catalyzed by CuxZn1-xS/RGO composite was investigated. The composites were characterized by X-ray diffraction (XRD), inductively coupled plasma-atomic emission spectrometer (ICP-AES), Fourier transform infrared spectroscopy (FTIR), ultraviolet-visible diffuse reflectance spectroscopy (UV-Vis), scanming electron microscopy (SEM) and transmission electron microscopy (TEM). The characterization results showed that spherical CuxZn1-xS nanoparticles were tightly attached to graphene. Doping of Cu2+ enhanced the response of CuxZn1-xS/RGO photocatalyst in the visible light range. The introduction of graphene inhibited the agglomeration of CuxZn1-xS nanoparticles and improved the photocatalytic performance. In addition, the photocatalytic degradation rate of Cu0.1Zn0.9S/RGO toward CIP was almost 8 times the rate of ZnS and 4.4 times that of Cu0.1Zn0.9S, respectively.
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Key words:
- photocatalytic /
- ciprofloxacin /
- CuxZn1-xS /
- graphene
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[1] MONDAL S K, SAHA A K, SINHA A. Removal of ciprofloxacin using modified advanced oxidation processes:Kinetics, pathways and process optimization[J]. Journal of Cleaner Production, 2018, 171:1203-1214. [2] MICHAEL I, RIZZO L, MCARDELL C S, et al. Urban wastewater treatment plants as hotspots for the release of antibiotics in the environment:A review[J]. Water Research, 2013, 47(3):957-995. [3] FUJISHIMA A, HONDA K. Electrochemical photolysis of water at a semiconductor electrode[J]. Nature, 1972, 238(58):37-38. [4] MURUGANANDHAM M, AMUTHA R, REPO E, et al. Controlled mesoporousself-assembly of ZnS microsphere for photocatalytic degradation of Methyl Orange dye[J]. J PhotochemPhotobio A, 2010, 216(2):133-141. [5] ZHANG Y, ZHANG N, TANG Z R, et al. Graphene transforms wide band gap ZnS to a visible light photocatalyst. The new role of graphene as a macromolecular photosensitizer[J]. Acs Nano, 2012, 6(11):9777-9789. [6] BOXI S S, PARIA S. Effect of silver doping on TiO2, CdS, and ZnS nanoparticles for the photocatalytic degradation of metronidazole under visible light[J]. Rsc Advances, 2014, 4(71):37752-37760. [7] MURUGANANDHAM M, AMUTHA R, REPO E, et al. Controlled mesoporous self-assembly of ZnS microsphere for photocatalytic degradation of Methyl Orange dye[J]. J Photochem Photobio A, 2010, 216(2):133-141. [8] ADELIFARD M, ESHGHI H. SYNTHESIS and characterization of nanostructural CuS-ZnS binary compound thin films prepared by spray pyrolysis[J]. Optic Commun 2012, 285(13):4400-4404. [9] 苏荣军, 薛雅内, 张广山, 等. Zn0.9Fe0.1S硫化物的制备及其光催化降解双酚A的性能[J]. 环境工程学报, 2017, 11(1):303-311. SU H J, XUE Y N, ZHANG G S, et al. Preparation of Zn0.9Fe0.1S sulfide and its photocatalytic degradation of bisphenol A[J]. Journal of Environmental Engineering,2017, 11(1):303-311(in Chinese).
[10] SUN X, DONG S, WANG E. One-step preparation and characterization of poly(propyleneimine) dendrimer-protected silver nanoclusters[J]. Macromolecules, 2004, 37(19):7105-7108. [11] BRIGHT K A, WILLIAMS C, KENWARD M A, et al. Antimicrobial action and efficiency of silver-loaded zeolite X[J]. Journal of Applied Microbiology, 2008, 104(5):1516-1524. [12] XU W P, ZHANG L C, LI J P, et al. Facile synthesis of silver@graphene oxide nanocomposites and their enhanced antibacterial properties[J]. Journal of Materials Chemistry, 2011, 21(12):4593-4597. [13] ZHANG Y, CUI W, AN W, et al. Combination of photoelectrocatalysis and adsorption for removal of bisphenol A over TiO2-graphene hydrogel with 3D network structure[J]. Applied Catalysis B:Environmental, 2018, 221:36-46. [14] KUMAR R, SINGH R K, SINGH D P, et al. Laser-assisted synthesis, reduction and micro-patterning of graphene:Recent progress and applications[J]. Coordination Chemistry Reviews, 2017, 342:34-79. [15] DONG C, LU J, QIU B, et al. Developing stretchable and graphene-oxide-based hydrogel for the removal of organic pollutants and metal ions[J]. Applied Catalysis B:Environmental, 2018, 222:146-156. [16] 蔡亭伟, 丁颖, 徐丽慧. 三维石墨烯材料在污水处理中的研究进展[J]. 环境化学, 2018, 37(6):1282-1292. CAI T W, DING Y, XU L H. Research progress of three-dimensional graphene materials in sewage treatment[J].Environmental Chemistry, 2018, 37(6):1282-1292(in Chinese).
[17] NI J, XUE J, SHEN J, et al. Fabrication of ZnAl mixed metal-oxides/RGO nanohybrid composites with enhanced photocatalytic activity under visible light[J]. Applied Surface Science, 2018, 441:599-606. [18] NI J, XUE J, XIE L F, et al. Construction of magnetically separable NiAl LDH/Fe3O4-RGO nanocomposites with enhanced photocatalytic performance under visible light[J]. Physical Chemistry Chemical Physics, 2017, 20(1):414-421. [19] LIANG J, WEI Y, ZHANG J, et al. Scalable green method to fabricate magnetically separable NiFe2O4-Reduced Graphene Oxide nanocomposites with enhanced photocatalytic performance driven by visible light[J]. Industrial & Engineering Chemistry Research, 2018, 57:4311-4319. [20] ZHU S R, QI Q, ZHAO W N, et al. Enhanced photocatalytic activity in hybrid composite combined BiOBr nanosheets and Bi2S3 nanoparticles[J]. Journal of Physics and Chemistry of Solids, 2018, 121:163-171. [21] 李鑫, 余长林, 樊启哲, 等. 溶剂热制备球状ZnS纳米光催化剂及其光催化性能[J]. 有色金属科学与工程, 2012, 3(3):21-26. LI X, YU C L, FAN Q Z, et al. Solvothermal preparation of spherical ZnS nano-photocatalyst and its photocatalytic properties[J].Science and Engineering of Non-Ferrous Metals, 2013, 3(3):21-26(in Chinese).
[22] 余长林, 李鑫, 周晚琴, 等. Al3+掺杂ZnS纳米晶的合成、表征及其光催化性能[J]. 人工晶体学报, 2013, 42(12):2620-2626. YU C L, LI X, ZHOU W Q, et al. Synthesis, characterization and photocatalytic activity of Al3+ doped zns nanocrystals[J].Journal of IOL, 2013, 42(12):2620-2626(in Chinese).
[23] JR W S H, OFFEMAN R E. Preparation of graphitic oxide[J]. J.Am.Chem.Soc, 1958, 80(6):1339. [24] GAO W, RAN C, WANG M, et al. The role of reduction extent of graphene oxide in the photocatalytic performance of Ag/AgX (X=Cl, Br)/rGO composites and the pseudo-secondorder kinetics reaction nature of the Ag/AgBrsystem[J]. Physical Chemistry Chemical Physics, 2016, 18(27):345-356. [25] CUI C, WANG Y, LIANG D, et al. Photo-assisted synthesis of Ag3PO4/reduced graphene oxide/Ag heterostructurephotocatalyst with enhanced photocatalytic activity and stability under visible light[J]. Applied Catalysis B:Environmental, 2014, 158-159(3):150-160. [26] BOXI S S, PARIA S. Effect of silver doping on TiO2, CdS, and ZnS nanoparticles for the photocatalytic degradation of metronidazole under visible light[J]. Rsc Advances, 2014, 4(71):37752-37760. [27] CHEN D, WEI X, HUANG Y. Preparation of ZnS quantum dots and photo-degradation of toxic organic pollutants[J]. Journal of China Three Gorges University, 2010, 32(2):92-102. [28] HE B, LIU R, REN J, et al. One-step solvothermal synthesis of petalous carbon-coated Cu+-doped CdS nanocomposites with enhanced photocatalytic hydrogen production[J]. Langmuir, 2017, 33, 6719-6726. [29] ZHAO Y, HE G, DAI W, et al. High catalytic activity in the phenol hydroxylation of magnetically separable CuFe2O4-reduced graphene oxide[J]. Industrial & Engineering Chemistry Research, 2014, 53(32):12566-12574. [30] QIU Q, CHEN Y, XUE J, et al. One-step solvothermal synthesis of spherical spinel type NiFe2-xMnxO4-RGO as high-performance supercapacitor electrodes[J]. Ceramics International, 2017, 43(2):2226-2232. [31] WANG L, CHEN H, XIAO L. CuS/ZnS hexagonal plates with enhanced hydrogen evolution activity under visible light irradiation[J]. Powder Technology, 2016, 288:103-108. -

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