吉林大学学报(地球科学版) ›› 2020, Vol. 50 ›› Issue (4): 1173-1181.doi: 10.13278/j.cnki.jjuese.20190060
• 地质工程与环境工程 • 上一篇
刘娜1,2, 张朋朋1,2, 丁隆真1,2, 陈红1,2, 焦昕倩1,2
Liu Na1,2, Zhang Pengpeng1,2, Ding Longzhen1,2, Chen Hong1,2, Jiao Xinqian1,2
摘要: 为了进一步研究氮掺杂碳材料活化过硫酸盐降解4-氯苯酚的方法,首先以廉价易得的废弃工业糖浆作为碳源,以氨水作为氮源,利用溶胶-凝胶法合成了3种氮掺杂碳材料(NC-700,NC-800和NC-900),并利用扫描电子显微镜(SEM)、X射线衍射(XRD)、拉曼光谱(Raman)、X射线光电子能谱(XPS)等技术对氮掺杂碳材料进行表征分析;然后考察了NC-800投加量、过硫酸盐(PDS)投加量和初始pH等因素对4-氯苯酚去除率的影响,并进行了电子自旋共振(ESR)和自由基淬灭实验。结果表明:3种材料均可有效活化PDS降解4-氯苯酚,其中NC-800活化PDS去除4-氯苯酚效率最高;当NC-800投加量为100 mg/L、PDS投加量为5 mmol/L时,反应30 min后,50 mg/L的4-氯苯酚的总去除率达99.10%;初始pH对4-氯苯酚去除率无明显影响;NC-800活化过硫酸盐降解4-氯苯酚遵循非自由基途径,单线态氧为降解4-氯苯酚的活性物质。循环使用实验证明NC-800具有一定的稳定性,4次循环使用后,4-氯苯酚去除率仍可达到73.80%。
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[1] Shukla P, Sun H, Wang S, et al. Nanosized Co3O4/SiO2 for Heterogeneous Oxidation of Phenolic Contaminants in Waste Water[J]. Separation and Purification Technology, 2011, 77(2):230-236. [2] Andreozzi R, Caprio V, Insola A, et al. Advanced Oxidation Processes (AOP) for Water Purification and Recovery[J]. Catalysis today, 1999, 53(1):51-59. [3] Esplugas S, Gimenez J, Contreras S, et al. Comparison of Different Advanced Oxidation Processes for Phenol Degradation[J]. Water Research, 2002, 36(4):1034-1042. [4] Ji K, Dai H, Deng J, et al. 3DOM BiVO4 Supported Silver Bromide and Noble Metals:High-Performance Photocatalysts for the Visible-Light-Driven Degradation of 4-Chlorophenol[J]. Applied Catalysis B:Environmental, 2015, 168:274-282. [5] 张凤君, 刘哲华, 苏小四,等. 土壤类型及组分对热活化过硫酸盐氧化降解土壤中挥发性氯代烃的影响[J]. 吉林大学学报(地球科学版), 2018, 48(4):1212-1220. Zhang Fengjun, Liu Zhehua, Su Xiaosi, et al. Effects of Soil Types and Composition on Oxidative Degradation of Volatile Chlorinated Hydrocarbons by Thermally Activated Persulfate[J]. Journal of Jilin University(Earth Science Edition), 2018, 48(4):1212-1220. [6] Wacławek S, Lutze H V, Grübel K, et al. Chemistry of Persulfates in Water and Wastewater Treatment:A Review[J]. Chemical Engineering Journal, 2017, 330:44-62. [7] Ghanbari F, Moradi M. Application of Peroxymonosulfate and Its Activation Methods for Degradation of Environmental Organic Pollutants[J]. Chemical Engineering Journal, 2017, 310:41-62. [8] Fang G, Gao J, Dionysiou D D, et al. Activation of Persulfate by Quinones:Free Radical Reactions and Implication for the Degradation of PCBs[J]. Environmental Science & Technology, 2013, 47(9):4605-4611. [9] Wacławek S, Antoš V, Hrabák P, et al. Remediation of Hexachlorocyclohexanes by Cobalt-Mediated Activation of Peroxymonosulfate[J]. Desalination and Water Treatment, 2016, 57(54):26274-26279. [10] Sun H, Peng X, Zhang S, et al. Activation of Peroxymonosulfate by Nitrogen-Functionalized Sludge Carbon for Efficient Degradation of Organic Pollutants in Water[J]. Bioresource Technology, 2017, 241:244-251. [11] Zhu C, Fang G, Dionysiou D D, et al. Efficient Transformation of DDTs with Persulfate Activation by Zero-Valent Iron Nanoparticles:A Mechanistic Study[J]. Journal of Hazardous Materials, 2016, 316:232-241. [12] 刘娜, 丁吉阳, 于庆民, 等. 超声强化零价铁活化过硫酸盐降解地下水中二恶烷[J]. 吉林大学学报(地球科学版), 2018, 48(6):1831-1837. Liu Na, Ding Jiyang, Yu Qingmin, et al. Degradation of 1,4-Dioxane in Groundwater by Ultrasound Enhanced ZVI Activated Persulfate Oxidation Process[J]. Journal of Jilin University(Earth Science Edition),2018, 48(6):1831-1837. [13] Ji Y, Fan Y, Liu K, et al. Thermo Activated Persulfate Oxidation of Antibiotic Sulfamethoxazole and Structurally Related Compounds[J]. Water Research, 2015, 87:1-9. [14] Zhang R, Yang Y, Huang C H, et al. Kinetics and Modeling of Sulfonamide Antibiotic Degradation in Wastewater and Human Urine by UV/H2O2 and UV/PDS[J]. Water Research, 2016, 103:283-292. [15] Rastogi A, Al-Abed S R, Dionysiou D D. Effect of Inorganic, Synthetic and Naturally Occurring Chelating Agents on Fe (Ⅱ) Mediated Advanced Oxidation of Chlorophenols[J]. Water Research, 2009, 43(3):684-694. [16] Oh W D, Dong Z, Lim T T. Generation of Sulfate Radical Through Heterogeneous Catalysis for Organic Contaminants Removal:Current Development, Challenges and Prospects[J]. Applied Catalysis B:Environmental, 2016, 194:169-201. [17] Duan X, Sun H, Shao Z, et al. Nonradical Reactions in Environmental Remediation Processes:Uncertainty and Challenges[J]. Applied Catalysis B:Environmental, 2018, 224:973-982. [18] Zhang T, Chen Y, Wang Y, et al. Efficient Peroxydisulfate Activation Process not Relying on Sulfate Radical Generation for Water Pollutant Degradation[J]. Environmental Science & Technology, 2014, 48(10):5868-5875. [19] Duan X, Sun H, Wang Y, et al. N-Doping-Induced Nonradical Reaction on Single-Walled Carbon Nanotubes for Catalytic Phenol Oxidation[J]. Acs Catalysis, 2014, 5(2):553-559. [20] Shi Q, Peng F, Liao S, et al. Sulfur and Nitrogen Co-doped Carbon Nanotubes for Enhancing Electrochemical Oxygen Reduction Activity in Acidic and Alkaline Media[J]. Journal of Materials Chemistry:A, 2013, 1(47):14853-14857. [21] Duan X, O'Donnell K, Sun H, et al. Sulfur and Nitrogen Co-Doped Graphene for Metal-Free Catalytic Oxidation Reactions[J]. Small, 2015, 11(25):3036-3044. [22] Han J S, Chung D Y, Ha D G, et al. Nitrogen and Boron Co-Doped Hollow Carbon Catalyst for the Oxygen Reduction Reaction[J]. Carbon, 2016, 105:1-7. [23] Xu J, Guan L. Toward Understanding the Active Site for Oxygen Reduction Reaction on Phosphorus-Encapsulated Single-Walled Carbon Nanotubes[J]. Rsc Advances, 2013, 3(16):5577-5582. [24] Sun H, Kwan C K, Suvorova A, et al. Catalytic Oxidation of Organic Pollutants on Pristine and Surface Nitrogen-Modified Carbon Nanotubes with Sulfate Radicals[J]. Applied Catalysis B:Environmental, 2014, 154:134-141. [25] Duan X, Ao Z, Sun H, et al. Nitrogen-Doped Graphene for Generation and Evolution of Reactive Radicals by Metal-Free Catalysis[J]. ACS Applied Materials & Interfaces, 2015, 7(7):4169-4178. [26] Hu P, Su H, Chen Z, et al. Selective Degradation of Organic Pollutants Using an Efficient Metal-Free Catalyst Derived from Carbonized Polypyrrole Via Peroxymonosulfate Activation[J]. Environmental Science & Technology, 2017,51(19):11288-11296. [27] Liu G, Liu Y, Zhang X, et al. Characterization and Catalytic Performance of Porous Carbon Prepared Using in Situ-Formed Aluminophosphate Framework as Template[J]. Journal of Colloid and Interface Science, 2010, 342(2):467-473. [28] Rao C V, Cabrera C R, Ishikawa Y. In Search of the Active Site in Nitrogen-Doped Carbon Nanotube Electrodes for the Oxygen Reduction Reaction[J]. The Journal of Physical Chemistry Letters, 2010, 1(18):2622-2627. [29] Vazquez-Santos M B, Geissler E, László K, et al. Graphitization of Highly Porous Carbons Derived from Poly (P-Phenylene Benzobisoxazole)[J]. Carbon, 2012, 50(8):2929-2940. [30] Ferrari A C, Basko D M. Raman Spectroscopy as a Versatile Tool for Studying the Properties of Graphene[J]. Nature Nanotechnology, 2013, 8(4):235-246. [31] Cheng Z, Pan Q, Rempel G L. Modification of Multiwall Carbon Nanotubes via Soap Free Emulsion Polymerization of Acrylonitrile[J]. Journal of Polymer Science:Part A:Polymer Chemistry, 2010, 48(10):2057-2062. [32] Long J, Xie X, Xu J, et al. Nitrogen-Doped Graphene Nanosheets as Metal-Free Catalysts for Aerobic Selective Oxidation of Benzylic Alcohols[J]. Acs Catalysis, 2012, 2(4):622-631. [33] Xu Y, Mo Y, Tian J, et al. The Synergistic Effect of Graphitic N and Pyrrolic N for the Enhanced Photocatalytic Performance of Nitrogen-Doped Graphene/TiO2 Nanocomposites[J]. Applied Catalysis B:Environmental, 2016, 181:810-817. [34] Liu N, Zhang L, Xue Y, et al. Nitrogen-Doped Carbon Material as a Catalyst for the Degradation of Direct Red 23 Based on Persulfate Oxidation[J]. Separation and Purification Technology, 2017, 184:213-219. [35] Duan X, Ao Z, Li D, et al. Surface-Tailored Nanodiamonds as Excellent Metal-Free Matalysts for Organic Oxidation[J]. Carbon, 2016, 103:404-411. [36] Hu P, Long M, Bai X, et al. Monolithic Cobalt-Doped Carbon Aerogel for Efficient Catalytic Activation of Peroxymonosulfate in Water[J]. Journal of Hazardous Materials, 2017, 332:195-204. [37] Yao Y, Chen H, Lian C, et al. Fe, Co, Ni Nanocrystals Encapsulated in Nitrogen-Doped Carbon Nanotubes as Fenton-Like Catalysts for Organic Pollutant Removal[J]. Journal of Hazardous Materials, 2016, 314:129-139. [38] Cheng X, Guo H, Zhang Y, et al. Non-Photochemical Production of Singlet Oxygen via Activation of Persulfate by Carbon Nanotubes[J]. Water Research, 2017, 113:80-88. |
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