TiO_2光催化降解去除土壤中荧蒽研究
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摘要
针对典型多环芳烃污染土壤,文章以荧蒽为目标污染物,选择TiO_2作为催化剂在紫外光照射下降解去除土壤中荧蒽,考察了降解时间、催化剂用量、搅拌次数以及土壤水分含量因素对降解率的影响,研究了腐殖酸和H_2O_2对荧蒽光催化降解率的影响,采用活性基团捕获实验探究了土壤中荧蒽的降解机理。结果表明:降解率随降解时间的增长而提高,其中P25用量为5%、降解时间为48 h时,降解率为24.11%;P25用量增加为20%,光照48 h后的降解率为42.89%;土壤搅拌可提高荧蒽降解效率,搅拌次数为5次时降解率为51.72%,与未搅拌相比提高了8.83%;加入10%的水分后,荧蒽降解率提高到56.90%。腐殖酸抑制荧蒽的降解,加入腐殖酸后降解率降低10.94%。加入1.5 mL质量分数30%的H_2O_2后降解率提高18.26%。加入对苯醌后荧蒽的降解率显著降低,表明·O_2~-在荧蒽的降解过程中起主要作用。
Aiming at the soil contaminated by polycyclic aromatic hydrocarbon,the fluoranthene was chosen as the targeted pollutant for degrading under irradiation of ultraviolet light,with TiO_2as catalyst.The effect of degradation time,catalyst dosage,stirring number and soil water content on degradation rate of fluoranthene were studied.The factors of humic acid and H_2O_2on the photocatalytic degradation of fluoranthene were explored.The degradation mechanism of fluoranthene in soil was investigated by adding trapping agents in the reaction system.The results showed that the degradation rate increased with the increase of degradation time.When the degradation rate of fluoranthene was 24.11%,the amount of P25 was 5%and the degradation time was 48 h,while when the amount of P25 increased to 20%,the degradation rate was 42.89%after 48 h.The degradation rate showed an upward trend with increasing stir times.The degradation rate was 51.72%after stir for 5 times,which was 8.83%higher than that without any stir.After adding 10%water,the degradation rate of fluoranthene reached 56.90%.However,it was inhibited by humic acid.The degradation rate could decrease by 10.94%after adding humic acid.The degradation rate increased by 18.26%after adding of 1.5 mL H_2O_2with a mass fraction of 30%.Adding p-quinone into reaction system could lead to a significant decrease of the degradation rate of fluoranthene,indicating that·O_2~-played a main role in the degradation process of fluoranthene.
Aiming at the soil contaminated by polycyclic aromatic hydrocarbon,the fluoranthene was chosen as the targeted pollutant for degrading under irradiation of ultraviolet light,with TiO_2as catalyst.The effect of degradation time,catalyst dosage,stirring number and soil water content on degradation rate of fluoranthene were studied.The factors of humic acid and H_2O_2on the photocatalytic degradation of fluoranthene were explored.The degradation mechanism of fluoranthene in soil was investigated by adding trapping agents in the reaction system.The results showed that the degradation rate increased with the increase of degradation time.When the degradation rate of fluoranthene was 24.11%,the amount of P25 was 5%and the degradation time was 48 h,while when the amount of P25 increased to 20%,the degradation rate was 42.89%after 48 h.The degradation rate showed an upward trend with increasing stir times.The degradation rate was 51.72%after stir for 5 times,which was 8.83%higher than that without any stir.After adding 10%water,the degradation rate of fluoranthene reached 56.90%.However,it was inhibited by humic acid.The degradation rate could decrease by 10.94%after adding humic acid.The degradation rate increased by 18.26%after adding of 1.5 mL H_2O_2with a mass fraction of 30%.Adding p-quinone into reaction system could lead to a significant decrease of the degradation rate of fluoranthene,indicating that·O_2~-played a main role in the degradation process of fluoranthene.
引文
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[19] Yin M C, Li Z S, Kou J H, et al. Mechanism investigation of visible light-induced degradation in a heterogeneous TiO2/eosin Y/Rhodamine B system[J]. Environmental Science and Technology, 2009,43(21):8361-8366.
[20] Chunmei L, Siyu Y, Hongjun D, et al. Z-scheme mesoporous photocatalyst constructed by modification of Sn3O4,nanoclusters on g-C3N4, nanosheets with improved photocatalytic performance and mechanism insight[J]. Applied Catalysis B:Environmental, 2018,238:284-293.
[2]陈星,宋昕,吕正勇,等. PAHs污染土壤的热修复可行性[J].环境工程学报, 2018,12(10):2833-2844.Chen Xing, Song Xin, Lyu Zhengyong, et al. Feasibility of thermal remediation of PAHs contaminated soil[J]. Journal of Environmental Engineering, 2018,12(10):2833-2844.
[3]麦天鹏.电化学修复荧蒽污染土壤试验研究[D].重庆：重庆大学, 2016.Mai Tianpeng. Experimental Study on Electrochemical Remediation of Fluoranthracene Contaminated Soil[D].Chongqing:Chongqing University, 2016.
[4]张惠灵,王宇,周杨,等.某焦化厂PM2.5中多环芳烃的排放特征及其对周边环境影响[J].环境工程学报, 2017,11(10):5571-5576.Zhang Huiling, Wang Yu, Zhou Yang, et al. Emission characteristics of PAHs in PM2.5of a coking plant and its impact on the surrounding environment[J]. Journal of Environmental Engineering, 2017,11(10):5571-5576.
[5] Wang Y S, Shen J H, Horng J J. Chromate enhanced visible light driven TiO2, photocatalytic mechanism on Acid Orange 7 photodegradation[J]. Journal of Hazardous Materials,2014,274(12):420-427.
[6]邓玲娟,古元梓,徐维霞,等.二氧化钛-石墨烯复合物的制备及其光催化性质[J].应用化学, 2012,29(8):942-947.Deng Lingjuan, Gu Yuanzi, Xu Weixia, et al. Preparation and photocatalytic properties of TiO2-graphene composites[J]. Applied Chemistry, 2012,29(8):942-947.
[7]刘子儒.表层土壤中部分多环芳烃的光化学降解研究[D].大连：大连理工大学, 2009.Liu Ziru. Photochemical Degradation of Some PAHs in Surface Soil[D]. Dalian:Dalian University of Technology, 2009.
[8] Wu R J, Chen C C, Chen M H, et al. Titanium dioxide-mediated heterogeneous photocatalytic degradation of terbufos:parameter study and reaction pathways[J]. Journal of Hazardous Materials, 2009,162(2):945-953.
[9] Dong D, Li P, Li X, et al. Photocatalytic degradation of phenanthrene and pyrene on soil surfaces in the presence of nanometer rutile TiO2, under UV-irradiation[J]. Chemical Engineering Journal, 2010,158(3):378-383.
[10] Qian X, Wu Y, Kan M, et al. FeOOH quantum dots coupled g-C3N4for visible light driving photo-Fenton degradation of organic pollutants[J]. Applied Catalysis B:Environmental, 2018,237:513-520.
[11] Dong D B, Li P J, Li X J, et al. Investigation on the photocatalytic degradation of pyrene on soil surfaces using nanometer anatase TiO2under UV irradiation[J].Journal of Hazardous Materials, 2010,174(1):859-863.
[12]陈静,黄占斌.腐植酸在土壤修复中的作用[J].腐植酸,2014(4):30-34,65.Chen Jing, Huang Zhanbin. The role of humic acid in soil remediation[J]. Humic Acid, 2014(4):30-34,65.
[13]郭佑罗,关小红,高乃云,等.紫外/过硫酸盐工艺降解水中氯贝酸的研究[J].中国环境科学, 2016,36(7):2014-2019.Guo Youluo, Guan Xiaohong, Gao Naiyun, et al. Degradation of chlorobenzic acid in water by UV/persulfate process[J]. Chinese Journal of Environmental Science, 2016,36(7):2014-2019.
[14] Miao X, Dai H, Chen J,et al. The enhanced method of hydroxyl radical generation in the heterogeneous UV-Fenton system withα-FeOOH as catalyst[J]. Separation and Purification Technology, 2018:S138358661733397X.
[15] Coleman H M, Vimonses V, Leslie G, et al. Degradation of1, 4-dioxane in water using TiO2based photocatalytic and H2O2/UV processes[J]. Journal of Hazardous Materials,2007,146(3):496-501.
[16] Wang Y, Tian H, Yu Y, et al. Enhanced catalytic activity ofα-FeOOH-rGO supported on active carbon fiber(ACF)for degradation of phenol and quinolone in the solar-Fenton system[J]. Chemosphere, 2018,43(3):317-324.
[17] Lisowski P, Colmenares J C, Ma?ek O, et al. Dual functionality of TiO2/biochar hybrid materials:photocatalytic phenol degradation in liquid phase and selective oxidation of methanol in gas phase[J]. ACS Sustainable Chemistry&Engineering, 2017.
[18] Khataee A, Kayan B, Gholami P, et al. Sonocatalytic degradation of an anthraquinone dye using TiO2-biochar nanocomposite[J]. Ultrasonics Sonochemistry, 2017,39(PtA):120.
[19] Yin M C, Li Z S, Kou J H, et al. Mechanism investigation of visible light-induced degradation in a heterogeneous TiO2/eosin Y/Rhodamine B system[J]. Environmental Science and Technology, 2009,43(21):8361-8366.
[20] Chunmei L, Siyu Y, Hongjun D, et al. Z-scheme mesoporous photocatalyst constructed by modification of Sn3O4,nanoclusters on g-C3N4, nanosheets with improved photocatalytic performance and mechanism insight[J]. Applied Catalysis B:Environmental, 2018,238:284-293.
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