Preparation of N-TiO2 photocatalyst and its degradation of organic pollutants under blue LED light
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摘要: 分别采用机械化学法、水解沉淀法和溶胶−凝胶法合成了氮掺杂二氧化钛（N-TiO2)催化剂，以亚甲基蓝（Methylene Blue, MB）和盐酸四环素（Tetracycline hydrochloride, TTC）为目标污染物. 光催化实验及催化剂的形貌表征对比表明，水解沉淀法合成的N-TiO2-H具有较高蓝光催化活性且颗粒分布均匀，无团聚现象. 选用N-TiO2-H进一步探讨煅烧温度、催化剂投加量、pH及降解底物初始浓度对光催化降解反应的影响. 研究表明，400 ℃煅烧下制备的N-TiO2-H具有最佳蓝光催化活性. 当反应pH=7时，0.5 g/L N-TiO2-H在460 nm蓝光照射下2 h可将初始浓度为5 mg/L的MB去除89.7%；当pH=5时，光照1.5 h可将初始浓度为50 mg/L的TTC，去除75.2%.Abstract: Nitrogen-doped titanium dioxide (N-TiO2) photocatalyst was synthesized by mechanochemical, hydrolysis precipitation and sol-gel method respectively. With the application of Methylene blue (MB) and tetraccycline hydrochloride (TTC) as the target pollutants, N-TiO2-H synthesized by hydrolysis precipitation method has high photocatalysis activity under blue LED irradiation, uniform particle distribution and no agglomeration. Therefore, N-TiO2-H was selected to study the effects of calcination temperature, catalyst dosage, pH and initial concentration of organic pollutants by photocatalysis. The results showed that N-TiO2-H calcined at 400 ℃ had the best photocatalytic activity under blue LED light irradiation. Under the dosage of 0.5 g/L N-TiO2-H, the photocatalytic degradation of MB with initial concentration of 5 mg/L, pH=7, MB removal was 89.7% after 2 h, and the photocatalytic degradation of TTC with initial concentration of 50 mg/L, pH=5, TTC removal was 75.2% after 1.5 h.
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图 5 制备方法对N-TiO2光催化降解有机污染物的影响
Figure 5. Effect of preparation methods on photocatalytic degradation of organic pollutants by N-TiO2
图 6 煅烧温度对N-TiO2-H光催化降解有机污染物的影响
Figure 6. Effects of calcination temperatures on photocatalytic degradation of organic pollutants by N-TiO2-H
图 7 投加量对N-TiO2-H光催化降解有机污染物的影响
Figure 7. Effect of dosage on photocatalytic degradation of organic pollutants by N-TiO2-H
图 8 溶液pH对N-TiO2-H光催化降解有机污染物的影响
Figure 8. Effect of solution pH on photocatalytic degradation of organic pollutants by N-TiO2-H
图 9 N-TiO2-H对不同浓度有机污染物降解的影响
Figure 9. Effect of N-TiO2-H on degradation of organic pollutants in different concentrations
图 10 重复使用N-TiO2-H对有机污染物降解的影响
Figure 10. Effect of reuse of N-TiO2-H on degradation of organic pollutants
表 1 实验试剂
Table 1. List of reagents
试剂名称 规格 供应单位 氨水（质量分数25%~28%） 分析纯，AR 上海泰坦科技股份有限公司 尿素 分析纯，AR 国药集团化学试剂有限公司 钛酸四丁酯 分析纯，AR 上海泰坦科技股份有限公司 无水乙醇 分析纯，AR 上海泰坦科技股份有限公司 硝酸 分析纯，AR 上海泰坦科技股份有限公司 TiO2（P25型） 纯度 ≥ 99.5% 德国Degussa有限公司 盐酸四环素（TTC） 分析纯，AR 阿拉丁试剂（上海）有限公司 亚甲基蓝（MB） 分析纯，AR 国药集团化学试剂有有限公司 
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[1] LI C, HONG Z, SHUAI W, et al. Removal of basic dye (methylene blue) from aqueous solution using zeolite synthesized from electrolytic manganese residue[J] . Journal of Industrial and Engineering Chemistry,2015,23:344 − 352. doi: 10.1016/j.jiec.2014.08.038 [2] 杜实之. 环境中的抗生素的残留、健康风险与治理技术综述[J] . 环境科学与技术,2021,44(9):37 − 38. [3] ZHANG J, ZHANG X, DONG S, et al. N-doped carbon quantum dots/TiO2 hybrid composites with enhanced visible light driven photocatalytic activity toward dye wastewater degradation and mechanism insight[J] . Journal of Photochemistry & Photobiology A: Chemistry,2016,325:104 − 110. [4] BAO L P, CHONG C O, SAHEED M, et al. Conventional and emerging technologies for removal of antibiotics from wastewater[J] . Journal of Hazardous Materials,2020,400:122961. doi: 10.1016/j.jhazmat.2020.122961 [5] 章丹. 二氧化钛光催化降解亚甲基蓝影响因素的研究[J] . 环境与发展,2019,31(7):3. doi: 10.16647/j.cnki.cn15-1369/X.2019.07.071 [6] LI X, PENG K, CHEN H, et al. TiO2 nanoparticles assembled on kaolinites with different morphologies for efficient photocatalytic performance[J] . Scientific Reports,2018,8:11663. [7] SIJIA, QIAN S, PU Y, et al. New insights on the enhanced non-hydroxyl radical contribution under copper promoted TiO2/GO for the photodegradation of tetracycline hydrochloride[J] . Journal of Environmental Sciences,2021,100(2):101 − 111. [8] 曹冬梅, 左翔, 袁丙青, 等. TiO2-Fe3O4复合催化剂对乳酸左氧氟沙星的光解研究[J] . 水处理技术,2018,44(3):4. [9] VAIANO V, SACCO O, SANNINO D, et al. Photocatalytic removal of spiramycin from wastewater under visible light with N-doped TiO2 photocatalysts[J] . Chemical Engineering Journal,2015,261:3 − 8. doi: 10.1016/j.cej.2014.02.071 [10] SACCO O, VAIANO V, DANIEL C, et al. Removal of phenol in aqueous media by N-doped TiO2 based photocatalytic aerogels[J] . Materials Science in Semiconductor Processing,2018,80:104 − 110. doi: 10.1016/j.mssp.2018.02.032 [11] PARIDA K M, PANY S, NAIK B. Green synthesis of fibrous hierarchical meso-macroporous N doped TiO2 nanophotocatalyst with enhanced photocatalytic H2 production[J] . International Journal of Hydrogen Energy,2013,38(9):3545 − 3553. doi: 10.1016/j.ijhydene.2012.12.118 [12] MAMBA G, MBIANDA X Y, Mishra A K. Photocatalytic degradation of the diazo dye naphthol blue black in water using MWCNT/Gd, N, S-TiO2 nanocomposites under simulated solar light[J] . Journal of Environmental Sciences,2015,33:219 − 228. doi: 10.1016/j.jes.2014.06.052 [13] GE J, SUN Y, CHEN W, et al. Z-scheme heterojunction based on NiWO4/WO3 microspheres with enhanced photocatalytic performance under visible light[J] . Dalton Transactions,2021,50:13801. doi: 10.1039/D1DT02558A [14] WANG J, SUN Y, WU C, et al. Enhancing photocatalytic activity of Bi2MoO6 via surface co-doping with Ni2 + and Ti4 + ions[J] . Journal of Physics and Chemistry of Solids,2019,129:209 − 216. doi: 10.1016/j.jpcs.2019.01.014 [15] HE F, MULIANE U, WEON S, et al. Substrate-specific mineralization and deactivation behaviors of TiO2 as an air-cleaning photocatalyst[J] . Applied Catalysis B:Environmental,2020,275:119145. doi: 10.1016/j.apcatb.2020.119145 [16] REDDAM H A, ELMAIL R, LLORIA S C, et al. Synthesis of Fe, Mn and Cu modified TiO2 photocatalysts for photodegradation of Orange II[J] . Boletin de la Sociedad Espanola de Ceramica y Vidrio,2020,59:138 − 148. doi: 10.1016/j.bsecv.2019.09.005 [17] TOUATI A, HAMMEDI T, NAJJAR W, et al. Photocatalytic degradation of textile wastewater in presence of hydrogen peroxide: Effect of cerium doping titania[J] . Journal of Industrial & Engineering Chemistry,2016,35:36 − 44. [18] FATTAHI A, ARLOS M J, BRAGG L M, et al. Photodecomposition of pharmaceuticals and personal care products using P25 modified with Ag nanoparticles in the presence of natural organic matter[J] . Science of The Total Environment,2021,752:142000. doi: 10.1016/j.scitotenv.2020.142000 [19] NDABANKULU V O, MADDILA S, JONNALAGADDA S B. Ozone facilitated degradation of caffeine using Ce-TiO2 catalyst[J] . Journal of Environmental Science and Health Part B,2018,54(2):1 − 9. [20] LI S, YANG Y, SU Q, et al. Synthesis and photocatalytic activity of transition metal and rare earth element co-doped TiO2 nano particles[J] . Materials Letters,2019,252:123 − 125. doi: 10.1016/j.matlet.2019.05.123 [21] WU D, LI C, ZHANG D H, et al. Enhanced photocatalytic activity of Gd3+ doped TiO2 and Gd2O3 modified TiO2 prepared via ball milling method[J] . Journal of Rare Earths,2019,37:845 − 852. doi: 10.1016/j.jre.2018.10.011 [22] SANCHEZ-MARTINEZ A, CEBALLOS-SANCHEZ O, KOOP-SANTA C, et al. N-doped TiO2 nanoparticles obtained by a facile coprecipitation method atlow temperature[J] . Ceramics International,2018,44:5273 − 5283. doi: 10.1016/j.ceramint.2017.12.140 [23] CHEN Y, LIU K. Preparation and characterization of nitrogen-doped TiO2/diatomite integrated photocatalytic pellet for the adsorption-degradation of tetracycline hydrochloride using visible light[J] . Chemical Engineering Journal,2016,302:682 − 696. doi: 10.1016/j.cej.2016.05.108 -
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