Modification of lead dioxide electrode and electrocatalytic degradation of anthracene in coking wastewater
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摘要: 为了研究电催化对焦化废水中污染物的降解效果,采用电沉积法制备了Ti/PbO2、Ti/PANI/PbO2和Ti/PANI/PbO2-Ce三种电极,对电极进行扫描电镜和X射线衍射表征、电化学性能测试、产羟基自由基(·OH)能力测试和加速寿命测试。结果表明,经聚苯胺(PANI)和铈(Ce)改性的Ti/PANI/PbO2-Ce电极具有更好的表面形貌和更高的催化活性,能产生更多的·OH,析氧电位为1.83 V,加速寿命时间为720 min。采用Ti/PANI/PbO2-Ce电极降解焦化废水中的蒽,考察了主要因素对降解效果的影响,得到蒽的最佳降解条件为电压14 V,板间距1.0 cm,电解质浓度0.35 mol/L,反应时间120 min,pH值10。Ti/PANI/PbO2-Ce电极显示了良好的电催化性能。Abstract: To investigate the electrocatalytic degradation effect of anthracene in coking wastewater, Ti/PbO2, Ti/PANI/PbO2 and Ti/PANI/PbO2-Ce electrodes were prepared by electrodeposition, and the electrodes were subjected to scanning electron microscopy and X-ray diffraction characterization, electrochemical performance test, hydroxyl radical (·OH) production capacity test and accelerated lifetime test.The results showed that the Ti/PANI/PbO2-Ce electrode modified with polyaniline (PANI) and cerium (Ce) had better surface morphology and higher catalytic activity, and could produce more ·OH with an oxygen precipitation potential of 1.83 V and an accelerated lifetime of 720 min.The Ti/PANI/PbO2-Ce electrode was used for the degradation of anthracene in coking wastewater, and the effects of the main factors on the degradation effect were investigated, and the optimal degradation conditions for anthracene were obtained as voltage 14 V, plate spacing of 1.0 cm, electrolyte concentration of 0.35 mol/L, reaction time of 120 min, pH value of 10.The Ti/PANI/PbO2-Ce electrode showed good electrocatalytic performance.
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Key words:
- electrocatalytic oxidation /
- polyaniline /
- cerium /
- hydroxyl radical /
- anthracene /
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表 1 某焦化企业废水中多环芳烃浓度
Table 1. Concentration of polycyclic aromatic hydrocarbons in wastewater from a coking enterprises
多环芳烃 浓度/(μg·L-1) 蒽 93.65 萘 73.64 苯并[a]蒽 56.72 菲 43.89 苯并[a]芘 37.55 芘 31.86 茚并[g,h,i]芘 26.54 苯并[k]荧蒽 23.87 -
[1] 刘伟. 高效菌强化OAO工艺处理焦化废水的试验研究[D]. 武汉科技大学, 2011.LIU Wei. Experimental Study on the application of highly effecive bacteria to enhance OAO process in treatment of coke plant wastewater[D]. Wuhan: Wuhan University of Science and Technology, 2011. [2] 王娟, 刘玉学, 范迪. 焦化废水深度处理试验研究[J]. 环境工程学报, 2009, 3(10): 1804-1807. https://www.cnki.com.cn/Article/CJFDTOTAL-HJJZ200910016.htmWANG Juan, LIU Yuxue, FAN Di. Experimental research on advanced treatment process of coking-plant wastewater[J]. Chinese Journal of Environmental Engineering, 2009, 3(10): 1804-1807. https://www.cnki.com.cn/Article/CJFDTOTAL-HJJZ200910016.htm [3] YANG W L, WANG J C, HUA M, et al. Characterization of effluent organic matter from different coking wastewater treatment plants[J]. Chemosphere, 2018, 203: 68-75. doi: 10.1016/j.chemosphere.2018.03.167 [4] QIN Z, WEI C, WEI T, et al. Evolution of biochemical processes in coking wastewater treatment: A combined evaluation of material and energy efficiencies and secondary pollution[J]. Science of the Total Environment, 2022, 807: 151072. doi: 10.1016/j.scitotenv.2021.151072 [5] 付江涛, 王黎, 王伟, 等. 焦化废水树脂吸附及深度处理回用[J]. 工业水处理, 2017, 37(5): 109-112. https://www.cnki.com.cn/Article/CJFDTOTAL-GYSC201705026.htmFU Jiangtao, WANG Li, WANG Wei, et al. Advancement treatment and reuse of coking wastewater by adsorption resin[J]. Industrial Water Treatment, 2017, 37(5): 109-112. https://www.cnki.com.cn/Article/CJFDTOTAL-GYSC201705026.htm [6] DU Z P, GONG Z P, QI W H, et al. Coagulation performance and floc characteristics of poly-ferric-titanium-silicate-chloride in coking wastewater treatment[J]. Colloids and Surfaces A-Physicochemical and Engineering Aspects, 2022, 642: 128413. [7] 齐文豪, 王淑军, 王旭明, 等. 聚硅酸铁钛絮凝剂制备及焦化废水混凝处理试验[J]. 净水技术, 2021, 40(4): 101-105, 120. https://www.cnki.com.cn/Article/CJFDTOTAL-ZSJS202104021.htmQI Wenhao, WANG Shujun, WANG Xuming, et al. Preparation of Polyferric Titanium Silicate Flocculant and the Experiment of Coagulation for Coking Wastewater Treatment[J]. Water Purification Technology, 2021, 40(4): 101-105, 120. https://www.cnki.com.cn/Article/CJFDTOTAL-ZSJS202104021.htm [8] FAN W L, SUN G X, WANG Q, et al. Identifying the critical activated carbon properties affecting the adsorption of effluent organic matter from bio-treated coking wastewater[J]. Science of the Total Environment, 2023, 871: 161968. doi: 10.1016/j.scitotenv.2023.161968 [9] CHOUDHARY R K, CHAUDHARI P K. Removal of pollutants of coking wastewater by adsorption[J]. Desalination and Water Treatment, 2017, 75: 45-57. doi: 10.5004/dwt.2017.20509 [10] 洪苡辰, 刘永泽, 张立秋, 等. 臭氧催化氧化深度处理焦化废水效能研究[J]. 给水排水, 2017, 53(12): 53-57. https://www.cnki.com.cn/Article/CJFDTOTAL-JZJS201712016.htmHONG Yichen, LIU Yongze, ZHANG Liqiu, et al. Advanced treatment of coking wastewater by catalytic ozonation[J]. Water & Wastewater Engineering, 2017, 53(12): 53-57. https://www.cnki.com.cn/Article/CJFDTOTAL-JZJS201712016.htm [11] GAO X Y, ZHANG H, WANG Y Q, et al. Study on preparation of a novel needle coke heterogeneous electro-Fenton cathode for coking wastewater treatment[J]. Chemical Engineering Journal, 2023, 455: 140696. doi: 10.1016/j.cej.2022.140696 [12] SHI W, LIU X J, LIU Y L, et al. Catalytic ozonation of hard COD in coking wastewater with Fe2O3/Al2O3-SiC: From catalyst design to industrial application[J]. Journal of Hazardous Materials, 2023, 447: 130759. doi: 10.1016/j.jhazmat.2023.130759 [13] 迟明超, 运晓静, 罗斌, 等. DSA电极的制备及应用的研究进展[J]. 应用化工, 2021, 50(2): 498-503. doi: 10.3969/j.issn.1671-3206.2021.02.048CHI Mingchao, YUN Xiaojing, LUO Bin, et al. Research progress on preparation and application of DSA electrode[J]. Applied Chemical Industry, 2021, 50(2): 498-503. doi: 10.3969/j.issn.1671-3206.2021.02.048 [14] BI Q, ZHANG Z K, SUN Y F, et al. Preparation and performance of highly active and long-life mesopore Ti/SnO2-Sb electrodes for electrochemical degradation of phenol[J]. Journal of Alloys and Compounds, 2021, 889: 161657. doi: 10.1016/j.jallcom.2021.161657 [15] DONG G H, DONG L LLANG K, et al. Insight into the high-efficient electrocatalytic elimination toward antibiotics via introducing FeTiO3 interlayer under Ce-PbO2 coating[J]. Journal of Environmental Chemical Engineering, 2022, 10(5): 108453. doi: 10.1016/j.jece.2022.108453 [16] LAN H, TAO Q B, MA N W, et al. Electrochemical oxidation of lamivudine using graphene oxide and Yb co-modified PbO2 electrodes: characterization, influencing factors and degradation mechanisms[J]. Separation and Purification Technology, 2022, 301: 121856. doi: 10.1016/j.seppur.2022.121856 [17] YAO Y W, REN B L, YANG Y, et al. Preparation and electrochemical treatment application of Ce-PbO2/ZrO2 composite electrode in the degradation of acridine orange by electrochemical advanced oxidation process[J]. Journal of Hazardous Materials, 2019, 361: 141-151. doi: 10.1016/j.jhazmat.2018.08.081 [18] 罗纲, 雷国元, 周达, 等. Ti/TiO2NTs/PANI/PbO2-CNTs电极的制备及煤气管道水封水的预处理[J]. 化工环保, 2022, 42(2): 184-189. https://www.cnki.com.cn/Article/CJFDTOTAL-HGHB202202009.htmLUO Gang, LEI Guoyuan, ZHOU Da, et al. Preparation of Ti/TiO2NTs/PANI/PbO2-CNTs electrode andpretreatment of water seal water of gas pipeline[J]. Environmental Protection of Chemical Industry, 2022, 42(2): 184-189. https://www.cnki.com.cn/Article/CJFDTOTAL-HGHB202202009.htm [19] 王燕, 赵瑞阳, 朱怀工, 等. 新型Ce掺杂Ti/SnO2-Sb电极的制备及其性能研究[J]. 现代化工, 2016, 36(11): 90-93, 95. https://www.cnki.com.cn/Article/CJFDTOTAL-XDHG201611022.htmWANG Yan, ZHAO Ruiyang, ZHU Huaigong, et al. Preparation of a novel Ce-doped Ti/SnO2-Sb electrode and its electro-catalytic performance[J]. Modern Chemical Industry, 2016, 36(11): 90-93, 95. https://www.cnki.com.cn/Article/CJFDTOTAL-XDHG201611022.htm [20] 张志军, 成鹏, 谢智翔, 等. 改性钛基二氧化铅电极催化氧化降解水中四环素[J]. 工业水处理, 2023, 43(3): 71-79. https://www.cnki.com.cn/Article/CJFDTOTAL-GYSC202303008.htmZHANG Zhijun, CHENG Peng, XIE Zhixiang, et al. Catalytic oxidation degradation of tetracycline in water by modified titanium-based lead dioxide electrode[J]. Industrial Water Treatment, 2023, 43(3): 71-79. https://www.cnki.com.cn/Article/CJFDTOTAL-GYSC202303008.htm [21] XU Z S, LIU H, NIU J F, et al. Hydroxyl multi-walled carbon nanotube-modified nanocrystalline PbO2 anode for removal of pyridine from wastewater[J]. Journal of Hazardous Materials, 2017, 327: 144-152. [22] 张传香, 何建平, 赵桂网, 等. 掺碳的钠离子电池正极材料NaVPO4F的电化学性能[J]. 无机化学学报, 2007, 23(4): 649-654. https://www.cnki.com.cn/Article/CJFDTOTAL-WJHX200704015.htmZHANG Chuanxiang, HE Jianping, ZHAO Guiwang, et al. Electrochemical Characteristics of C-doped NaVPO4F Cathode Material for Sodium-ion Battery[J]. Chinese Journal of Inorganic Chemistry, 2007, 23(4): 649-654. https://www.cnki.com.cn/Article/CJFDTOTAL-WJHX200704015.htm [23] PERIYASAMY S, MUTHUCHAMY M. Electrochemical oxidation of paracetamol in water by graphite anode: Effect of pH, electrolyte concentration and current density[J]. Journal of Environmental Chemical Engineering, 2018, 6(6): 7358-7367. [24] TAN C, XIANG B, LI Y J, et al. Preparation and characteristics of a nano-PbO2 anode for organic wastewater treatment[J]. Chemical Engineering Journal, 2011, 166(1): 15-21. [25] 倪智丽. Nd掺杂钛基PbO2电极制备及降解双酚S研究[D]. 杭州: 浙江大学, 2020.NI Zhili. The preparation of Nd doped PbO2 electrodes and the electrochemical oxidation of BPS[D]. Hangzhou: Zhejiang University, 2020. [26] SHIN Y U, YOO H Y, AHN Y Y, et al. Electrochemical oxidation of organics in sulfate solutions on boron-doped diamond electrode: Multiple pathways for sulfate radical generation[J]. Applied Catalysis B-Environmental, 2019, 254: 156-165. [27] 束蒋成. 改性钛基二氧化铅电极电化学降解水中四环素的研究[D]. 常州: 常州大学, 2022.SHU Jiangcheng. Electrochemical degradation of tetracycline in water by modified titanium based lead dioxide electrode[D]. CHangzhou: Changzhou University, 2022. [28] XIE J, YANG H Z, WANG X Q, et al. ZIF-8/electro-reduced graphene oxide nanocomposite for highly electrocatalytic oxidation of hydrazine in industrial wastewater[J]. Microchemical Journal, 2021, 168: 106521. [29] NIU J F, LI Y, SHANG E X, et al. Electrochemical oxidation of perfluorinated compounds in water[J]. Chemosphere, 2016, 146: 526-538.