高压脉冲放电降解4-氯酚废水的实验研究
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摘要
采用多针-板高压脉冲气液两相放电反应系统处理难降解的4-氯酚废水,并运用控制变量方法确定多种工艺参数的最佳值。考察了中间产物浓度变化情况、溶液矿化率、总有机碳浓度(TOC),并对4-氯酚的降解过程进行分析研究。实验结果表明:在脉冲电压26 kV、脉冲频率70 Hz、电极间距1.0 cm、曝气量4 L/min的情况下,150 mg/L的4-氯酚废水溶液放电处理90 min后降解率为67.25%。在放电过程中溶液导电性较高对活性粒子的生成有抑制作用导致溶液矿化率较低。整个放电过程中,溶液TOC整体呈缓慢下降趋势,中间产物浓度先增大后减小,其中峰值浓度最高的是4-氯邻苯二酚,峰值浓度最低的是对苯酚。
The refractory 4-chlorophenol wastewater was treated by multi-needle-plate high-pressure pulse gas-liquid two-phase discharge reaction system, and the optimal value of various process parameters was determined by using the control variable method. With changing the intermediate product concentration, solution mineralization rate and total organic carbon concentration(TOC), the degradation process of 4-chlorophenol was analyzed and inferred. The experimental results show in the following circumstances, the degradation rate of 150 mg/L of 4-chlorophenol wastewater treatment can reach 67.25% after 90 min discharge process: the pulse voltage at 26 kV, pulse frequency at 70 Hz, electrode spacing at 1.0 cm, and aeration at 4 L/min. In the discharge process, the high conductivity of the solution has the inhibitory effect on the generation of the active particles, which leads to the lower solution mineralization rate. During the whole discharge process, the solution TOC showed a slow downward trend. The concentration of intermediate products increases first and then decreases. Among the peak concentration, the highest is 4-chloro-o-phenol and the lowest is phenol.
The refractory 4-chlorophenol wastewater was treated by multi-needle-plate high-pressure pulse gas-liquid two-phase discharge reaction system, and the optimal value of various process parameters was determined by using the control variable method. With changing the intermediate product concentration, solution mineralization rate and total organic carbon concentration(TOC), the degradation process of 4-chlorophenol was analyzed and inferred. The experimental results show in the following circumstances, the degradation rate of 150 mg/L of 4-chlorophenol wastewater treatment can reach 67.25% after 90 min discharge process: the pulse voltage at 26 kV, pulse frequency at 70 Hz, electrode spacing at 1.0 cm, and aeration at 4 L/min. In the discharge process, the high conductivity of the solution has the inhibitory effect on the generation of the active particles, which leads to the lower solution mineralization rate. During the whole discharge process, the solution TOC showed a slow downward trend. The concentration of intermediate products increases first and then decreases. Among the peak concentration, the highest is 4-chloro-o-phenol and the lowest is phenol.
引文
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[20] SUN B, SATO M, CLEMENTS J S. Optical study of active species produced by a pulsed streamer corona discharge in water[J]. J Electrostatics, 1997,39(3):189-202.
[2] 李啸乾, 王国英, 王慧礼, 等. 波茨坦短芽孢杆菌降解4-氯酚和苯酚的特性[J]. 安全与环境学报, 2016,16(6):252-6.
[3] 王岩, 施钦, 王辉, 等. 电化学还原-氧化工艺降解4-氯酚的毒性研究[J]. 环境科学, 2016(4):1437-1443.
[4] 方梦祥,姚鹏,岑建孟,等. 活性炭吸附处理含酚废水的研究进展[J]. 化工进展, 2018,37(2):744-50.
[5] 唐建军, 邓爱华. TiO2光催化降解水溶液中的4-氯苯酚[J]. 应用化工, 2006,35:924-926.
[6] WANG Qing, LI Yi, LI Jing, et al. Experimental and kinetic study on the cometabolic biodegradation of phenol and 4-chlorophenol by psychrotrophic Pseudomonas putida LY1[J]. Environmental Science & Pollution Research, 2015,22:565-573.
[7] JOSHI A A, LOCKE B R, ARCE P, et al. Formation of hydroxyl radicals, hydrogen peroxide and aqueous elec-trons by pulsed streamer corona discharge in aqueous solution[J]. J Hazardous Materials, 1995,41(1):3-30.
[8] 闫克平. 高电压环境工程应用研究关键技术问题分析及展望[J]. 高压电技术, 2015,41(8):2528-2544.
[9] STRATTAN G R, DAI F, BELLONA C L, et al. Plasma-based water treatment: Efficient transformation of perfluoroalkyl substances (PFASs) in prepared solutions and contaminated groundwater[J]. Environmental Science & Technology, 2017,51:1643-1648.
[10] 张延宗, 郑经堂, 陈宏刚. 高压脉冲放电水处理技术的理论研究[J]. 高电压技术, 2007(2):136-140.
[11] 孙明, 金宏力, 杨颜颜, 等. 脉冲放电等离子体协同二氧化钛降解偶氮类染料废水[J]. 高电压技术, 2015(9):2862-2867.
[12] SUGIARTO A T. Pulsed plasma processing of organic compounds in aqueous solution[J]. Thin Solid Films, 2001, 386(2):295-299.
[13] HOEBEN W, VELDHUIZEN E, RUTGERS W, et al. The degradation of aqueous phenol solutions by pulsed positive corona discharges[J]. Plasma Sources Science & Technology, 2000,9(3):361.
[14] 胡祺昊, 王黎明, 黄兴华, 等. 高压脉冲放电降解染料废水的实验研究[J]. 清华大学学报:自然科学版, 2002,42(9):1148-1150.
[15] 董冰岩, 张鹏, 聂亚林, 等. 针-板式高压脉冲气液两相放电降解废水中的苯酚[J]. 化工进展, 2016,35(1):314-319.
[16] 董冰岩, 邓苇, 孙宇, 等. 高压脉冲放电协同纳米催化剂降解苯酚废水[J]. 高电压技术, 2017,43(8):2645-4652.
[17] WILLBERG D M, LANG P S, HOCHEMER R H, et al. Degradation of 4-chlorophenol,3,4-dichloroaniline, and 2,4,6-trinitrotoluene in an electrohydraulic discharge reactor [J]. Environ Sci Technol, 1996,30:2526-2534.
[18] 陈银生, 张新胜, 袁渭康. 高压脉冲放电低温等离子体法降解废水中4-氯酚[J]. 华东理工大学学报:自然科学版, 2002,28(3):232-234.
[19] YAO S L, SUZUKI E, NAKAYAMA A. Influence of rise time of pulse voltage on the pulsed plasma conversion of methane[J]. Energy Fuels, 2001,15(5):1300-1303.
[20] SUN B, SATO M, CLEMENTS J S. Optical study of active species produced by a pulsed streamer corona discharge in water[J]. J Electrostatics, 1997,39(3):189-202.