Research on the oxidative degradation of 2,4-dichlorophenol in water by Fe0-CNTs-Cu activation
PAN Jia-min1, GONG Xiao-bo1,2, CHEN Yong1, CHEN Liu1, LIU Yong1,2
1. College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610066, China; 2. Key Laboratory of Special Waste Water Treatment, Sichuan Province Higher Education System, Chengdu 610066, China
Abstract:In order to efficiently remove chlorophenols pollutants from wastewater, which are persistent, highly toxic and difficult to biodegrade, a new material (Fe0-CNTs-Cu) that could efficiently and selectively reduce oxygen to H2O2 and decompose the in-situ H2O2 to ·OH/O2·- was prepared by high energy ball milling-high temperature melting-liquid phase reduction method. The degradation mechanism of Fe0-CNTs-Cu/O2 system was analysed, and the degradation pathway of 4-CP in this system was speculated. The degradation rate and TOC removal rate of Fe0-CNTs-Cu for 2,4-dichlorophenol (2,4-DCP) under the optimized conditions were 92.3% and 54.2%, respectively. In the Fe0-CNTs-Cu/O2 system, a corrosion cell was formed to induce the selective reduction of O2 on the surface of CNTs to H2O2, Cu0, Cu2O and CNTs as well as the in situ generated Fe2+. The in situ generated H2O2 was catalytically decomposed to the highly oxidized material ·OH/O2·-, which could efficiently oxidatively degrade 2,4-DCP.
潘嘉敏, 龚小波, 陈勇, 陈柳, 刘咏. Fe0-CNTs-Cu活化O2降解水中2,4-二氯苯酚[J]. 中国环境科学, 2021, 41(6): 2657-2664.
PAN Jia-min, GONG Xiao-bo, CHEN Yong, CHEN Liu, LIU Yong. Research on the oxidative degradation of 2,4-dichlorophenol in water by Fe0-CNTs-Cu activation. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(6): 2657-2664.
潘煜,孙力平,陈星宇,等. CMC改性纳米Fe/Cu双金属模拟PRB去除地下水中2,4-二氯苯酚[J]. 中国环境科学, 2019,39(9):3789-3796. Pan Y, Sun L P, Chen X Y, et al. Removal of 2,4-dichlorophenol from groundwater by PRB simulated by CMC modified nanoscale Fe/Cu bimetal[J]. China Environmental Science, 2019,39(9):3789-3796.
[2]
张永祥,常杉,李飞,等.稳定型纳米零价铁去除地下水中2,4-二氯苯酚[J]. 环境科学, 2017,38(6):2385-2392. Zhang Y X, Chang S, Li F, et al. Removal of 2,4-dichlorophenol in underground water by stabilized nano zerovalent iron[J]. Environmental Science, 2017,38(6):2385-2392.
[3]
田凯勋,杨超,肖泉,等.超声强化零价铁/过硫酸钾体系降解2,4,6-三氯苯酚废水[J]. 中国环境科学, 2017,37(10):3729-3734. Tian K X, Yang C, Xiao Q, et al. Degradation of 2,4,6-TCP in an ultrasound-enhanced zero-valent iron/potassium persulfate system[J]. China Environmental Science, 2017,37(10):3729-3734.
[4]
潘煜,孙力平,张婷婷,等.CMC改性的纳米Fe/Cu双金属去除2,4-二氯苯酚的研究[J]. 环境科学学报, 2019,39(4):1174-1182. Pan Y, Sun L P, Zhang T T, et al. Study on removal of 2,4-dichlorophenol by CMC modified nanoscale Fe/Cu bimetal[J]. Acta Scientiae Circumstantiae, 2019,39(4):1174-1182.
[5]
Zhang M, Dong H, Zhao L, et al. A review on Fenton process for organic wastewater treatment based on optimization perspective[J]. Science of The Total Environment, 2019,670:110-121.
[6]
Zhang Y, Zhou M. A critical review of the application of chelating agents to enable Fenton and Fenton-like reactions at high pH values[J]. Journal of Hazardous Materials, 2019,362:436-450.
[7]
姚宏,向鑫鑫,薛宏慧,等.紫外光芬顿-膜分离耦合体系降解金霉素[J]. 中国环境科学, 2020,40(4):1577-1585. Yao H, Xiang X X, Xue H H, et al. Study on degradation of chlortetracycline by photo-Fenton ceramic membrane coupling system[J]. China Environmental Science, 2020,40(4):1577-1585.
[8]
潘心宇,王娅茹,刘凯,等.半胱氨酸强化针铁矿类芬顿反应降解2,4-二氯苯酚及影响因素[J]. 生态环境学报, 2020,29(1):207-214. Pan X Y, Wang Y R, Liu K, et al. Degradation of 2, 4-dichlorophenol by cysteine-enhanced goethite fenton-like reaction and its influencing factors[J]. Ecology and Environmental Sciences, 2020,29(1):207-214.
[9]
陈禹彤,张秀芳,田世超,等.阴极原位产H2O2强化光电催化降解水中EDTA的研究[J]. 环境科学学报, 2017,37(3):971-976. Chen Y T, Zhang X F, Tian S C, et al. In-situ generation of H2O2 in cathode to enhance the photoelectrocatalytic degradation of EDTA in water[J]. Acta Scientiae Circumstantiae, 2017,37(3):971-976.
[10]
Chung T H, Meshref M N A, Hai F I, et al. Microbial electrochemical systems for hydrogen peroxide synthesis:Critical review of process optimization, prospective environmental applications, and challenges[J]. Bioresource Technology, 2020,313:123727.
[11]
Gong X, Yang Z, Peng L, et al. In-situ synthesis of hydrogen peroxide in a novel Zn-CNTs-O2system[J]. Journal of Power Sources, 2018,378:190-197.
[12]
Yang Z, Gong X, Wang B, et al. Efficient in situ generation of H2O2 by novel magnesium-carbon nanotube composites[J]. RSC Advances, 2018,8(61):35179-35186.
[13]
Liu Y, Tan N, Guo J, et al. Catalytic activation of O2by Al0-CNTs-Cu2O composite for Fenton-like degradation of sulfamerazine antibiotic at wide pH range[J]. Journal of Hazardous Materials, 2020, 396:122751.
[14]
Chen Y, Yang Z, Liu Y, et al. Fenton-like degradation of sulfamerazine at nearly neutral pH using Fe-Cu-CNTs and Al0-CNTs for in-situ generation of H2O2/OH/O2-[J]. Chemical Engineering Journal, 2020,396:125329.
[15]
Chenakin S, Kruse N. XPS characterization of transition metal oxalates[J]. Applied Surface Science, 2020,515:146041.
[16]
徐斌,张书陵,高月香,等.石墨烯三维电极-电Fenton系统降解甲基橙[J]. 中国环境科学, 2020,40(10):4385-4394. Xu B, Zhang S L, Gao Y X, et al. Degradation of methyl orange by graphene three-dimensional electrode-electro Fenton system[J]. China Environmental Science, 2020,40(10):4385-4394.
[17]
Xu L, Yang Y, Li W, et al. Three-dimensional macroporous graphene-wrapped zero-valent copper nanoparticles as efficient micro-electrolysis-promoted Fenton-like catalysts for metronidazole removal[J]. Science of the Total Environment, 2019,658:219-233.
[18]
Feng Y, Lee P, Wu D, et al. Degradation of contaminants by Cu+-activated molecular oxygen in aqueous solutions:Evidence for cupryl species (Cu3+)[J]. Journal of Hazardous Materials, 2017,331:81-87.
[19]
An X, Tang Q, Lan H, et al. Polyoxometalates/TiO2 Fenton-like photocatalysts with rearranged oxygen vacancies for enhanced synergetic degradation[J]. Applied Catalysis B:Environmental, 2019, 244:407-413.
[20]
Yang Z, Gong X, Peng L, et al. Zn0-CNTs-Fe3O4 catalytic in situ generation of H2O2 for heterogeneous Fenton degradation of 4-chlorophenol[J]. Chemosphere, 2018,208:665-673.
[21]
Zhang C, Zhou M, Ren G, et al. Heterogeneous electro-Fenton using modified iron-carbon as catalyst for 2,4-dichlorophenol degradation:Influence factors, mechanism and degradation pathway[J]. Water Research, 2015,70:414-424.