MXene/PMS利用EDTA-Cu催化降解EDTA-Cd性能与机理

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摘要在不添加低价态过渡金属条件下,MXene/PMS利用乙二胺四乙酸铜(EDTA-Cu)实现了乙二胺四乙酸镉(EDTA-Cd)的高效降解和Cd的回收.EDTA-Cd和总Cd在30min内的去除率达到80%和95%.增加MXene、PMS和Cu²⁺浓度均显著增强了EDTA-Cd和总Cd的去除.反应体系主要活性物种是羟基自由基(HO^·)和硫酸根自由基(SO₄^·-).在pH值 3.0~9.0范围内保持了优异的性能,对Cl^-、HCO₃^-、HPO₄^2-和腐殖酸具有良好的耐受性.MXene活化PMS将EDTA-Cu氧化破络,释放出游离Cu离子,并触发Cu(II)/Cu(I)价态循环,强化了PMS的活化,从而实现了EDTA-Cu/Cd的高效降解.MXene对Cu和Cd离子具有优异的吸附能力,实现了重金属的回收.本研究利用重金属络合物本身含有的过渡金属,开发了一种同步实现重金属络合物氧化破络与重金属回收的方法.

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	宋浩然
	徐一航
	陈龙雨
	赵群
	李晨
	曹妍
	张林丰
	胡学伟
	刘树根
	李英杰
	李杰
	田森林

关键词 ：重金属络合物, Mxene, 单过硫酸盐, Cu(II)/Cu(I)循环

Abstract：Without the addition of low-valent transition metals, MXene/PMS achieved efficient degradation of EDTA-Cd and recovery of Cd using copper ethylenediaminetetraacetate (EDTA-Cu). The removal efficiency of EDTA-Cd and total Cd reached 80% and 95% within 30minutes, respectively. Increasing the concentrations of MXene, PMS, and Cu² significantly enhanced the removal of EDTA-Cd and total Cd. The primary reactive species in reaction process were identified as hydroxyl radical (HO^·) and sulfate radical (SO₄^·-). Excellent performance was maintained within a pH range of 3.0 to 9.0, with good resistance to Cl^-, HCO₃^-, HPO₄^2-, and humic acid. Activation of PMS by MXene initiated the oxidative decomposition of EDTA-Cu and released free Cu ions. Then, MXene triggered the Cu(II)/Cu(I) cycle and furtherly enhanced PMS activation, and thereby achieved the efficient degradation of EDTA-Cu/Cd. Additionally, MXene exhibited excellent adsorption capacity for Cu and Cd ions, thus to achieve the recovery of heavy metals. This study utilized the transition metals inherent in heavy metal complexs to develop an efficient method that simultaneously achieves the oxidative decomplexation of heavy metal complexes and the recovery of heavy metals.

Key words： heavy metal complexes Mxene PMS Cu(II)/Cu(I) cycle

收稿日期: 2024-05-21

PACS:

X703

基金资助:国家自然科学基金(52100077,22366024,22366022),广东省基础与应用基础研究基金(2020A1515410002)

通讯作者: 田森林,教授,tiansenlin@outlook.com E-mail: tiansenlin@outlook.com

作者简介: 宋浩然(1989-),男,河南许昌人,教授,博士,研究方向为多介质污染控制化学与关键技术.发表论文30余篇.shr3478@126.com.

引用本文:

宋浩然, 徐一航, 陈龙雨, 赵群, 李晨, 曹妍, 张林丰, 胡学伟, 刘树根, 李英杰, 李杰, 田森林. MXene/PMS利用EDTA-Cu催化降解EDTA-Cd性能与机理[J]. 中国环境科学, 2024, 44(12): 6729-6740. SONG Hao-ran, XU Yi-hang, CHEN Long-yu, ZHAO Qun, LI Chen, CAO Yan, ZHANG Lin-feng, HU Xue-wei, LIU Shu-gen, LI Ying-jie, LI Jie, TIAN Sen-lin. Catalytic degradation of EDTA-Cd by EDTA-Cu in MXene/PMS process: Performance and mechanism. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(12): 6729-6740.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2024/V44/I12/6729

[1] Wang Q, Li Y, Liu Y, et al. Effective removal of the heavy metal- organic complex Cu-EDTA from water by catalytic persulfate oxidation: Performance and mechanisms [J]. Journal of Cleaner Production, 2021,314,128119.
[2] Zhang H, Zhang R, Lu T, et al. Enhanced transport of heavy metal ions by low-molecular-weight organic acids in saturated porous media: Link complex stability constants to heavy metal mobility [J]. Chemosphere, 2022,290,133339.
[3] Korhonen M S, Muscarine S E, Tuhkanen T A. Removal of ethylenediaminetetraacetic acid (EDTA) from pulp mill effluents by ozonation [J]. Ozone: Science & Engineering, 2000,22(3):279- 286,279.
[4] Cuprys A, Pulicharla R, Lecka J, et al. Ciprofloxacin-metal complexes -stability and toxicity tests in the presence of humic substances [J]. Chemosphere, 2018,202:549-559.
[5] 王悦,杜小雨,黄鑫,等.废水中重金属离子的处理方法及研究现状[J]. 印染, 2023,49(9):91-96. Wang Y, Du X Y, Huang X, et al. Treatment methods and research status of heavy metal ions in wastewater [J]. China Dyeing & Finishing, 2023,49(9):91-96.
[6] 路永正,阎百兴.微生物对沉积物主要化学组分吸附重金属能力的影响[J]. 中国环境科学, 2011,31(1):105-110. Lu Y Z, Yan B X. Effect of microorganisms on adsorption capacities of Pb and Cd on main chemical components in sediments [J]. China Environmental Science, 2011,31(1):105-110.
[7] Lin L C, Li J K, Juang R S. Removal of Cu (II) and Ni(II) from aqueous solutions using batch and fixed-bed ion exchange processes [J]. Desalination, 2008,225(1-3):249-259,249.
[8] 陈聪.电催化臭氧氧化降解重金属络合物与金属同步回收特性与机理[D]. 温州:温州大学, 2022. Chen C. Performance and mechanism of decomplexation of metal- organic complexes and simultaneous recovery of metals by electrolysis-O₃and electro-peroxone [D]. Wenzhou: Wenzhou University, 2022.
[9] Xu Z, Wu T, Cao Y, et al. Efficient decomplexation of heavy metal- EDTA complexes by Co²⁺/peroxymonosulfate process: The critical role of replacement mechanism [J]. Chemical Engineering Journal, 2020,392,123639.
[10] Xu Z, Gao G, Pan B, et al. A new combined process for efficient removal of Cu (II) organic complexes from wastewater: Fe (III) displacement/UV degradation/alkaline precipitation [J]. Water Research, 2015,87:378-384.
[11] Liu Y, Wang D, Xue M, et al. High-efficient decomplexation of Cu-EDTA and Cu removal by high-frequency non-thermal plasma oxidation/alkaline precipitation. Separation and Purification Technology [J]. 2021,257,117885.
[12] Cao Y, Qian X C, Zhang Y X, et al. Decomplexation of EDTA- chelated copper and removal of copper ions by non-thermal plasma oxidation/alkaline precipitation [J]. Chemical Engineering Journal, 2019,362:487-496.
[13] Naguib M, Kurtoglu M, Presser V, et al. Two-dimensional nanocrystals produced by exfoliation of Ti₃AlC₂ [J]. Advanced Materials. 2011,23(37):4248-4253.
[14] 韩亚南,洪家辉,张安睿,等.MXene二维无机材料在环境修复中的应用[J]. 化学进展, 2022,(5):1229-1244. Han Y N, H J H, Z A R, et al. A review on MXene and its applications in environmental remediation [J]. Progress in Chemistry, 2022,(5):1229-1244.
[15] Song H R, Zu D, Li C, et al. Ultrafast activation of peroxymonosulfate by reduction of trace Fe³⁺ with Ti₃C₂MXene under neutral and alkaline conditions: Reducibility and confinement effect [J]. Chemical Engineering Journal, 2021,423,130012,130012.
[16] Shahzad A, Rasool K, Miran W, et al. Two-dimensional Ti₃C₂T_X MXene nanosheets for efficient copper removal from water [J]. ACS Sustainable Chemical Engineering Journal. 2017,5(12):11481-11488.
[17] Peng Q, Guo J, Zhang Q, et al. Unique lead adsorption behavior of activated hydroxyl group in two-dimensional titanium carbide [J]. Journal of the American Chemical Society, 2014,136(11):4113-4116.
[18] Ying Y, Liu Y, Wang X, et al. Two-dimensional titanium carbide for efficiently reductive removal of highly toxic chromium (VI) from water [J]. ACS Applied Materials & Interfaces, 2015,7(3):1795-1803.
[19] Shahzad A, Rasool K, Miran W, et al. Mercuric ion capturing by recoverable titanium carbide magnetic nanocomposite [J]. Journal of Hazardous Materials, 2018,344:811-818.
[20] Ding M, Chen W, Xu H, et al. Novel α-Fe₂O₃/MXene nanocomposite as heterogeneous activator of peroxymonosulfate for the degradation of salicylic acid [J]. Journal of Hazardous Materials, 2020,382: 121064.
[21] Liu Y, Luo R, Li Y, et al. Sandwich-like Co₃O₄/MXene composite enhanced catalytic performance for Bisphenol A degradation [J]. Chemical Engineering Journal, 2018,347:731-740.
[22] Alhabeb M, Maleski K, Anasori B, et al. Guidelines for synthesis and processing of two-dimensional titanium carbide (Ti₃C₂T_X MXene) [J]. Chemistry of Materials. 2017,29(18):7633-7644.
[23] Zeng H, Liu S, Chai B, et al. Enhanced photoelectrocatalytic decomplexation of Cu-EDTA and Cu recovery by persulfate activated by UV and cathodic reduction [J]. Environmental Science & Technology, 2016,50(12):6459-6466.
[24] Huang X F, Xu Y, Shan C, et al. Coupled Cu(II)-EDTA degradation and Cu(II) removal from acidic wastewater by ozonation: Performance, products and pathways [J]. Chemical Engineering Journal, 2016,299: 23-29.
[25] Zhang Y, Wang J, Yang Z, et al. Hydrazine hydrate accelerates neocuproine-copper complex generation and utilization in alkyne reduction, a significant supplement method for catalytic hydrogenation [J]. Journal of Organic Chemistry, 2021,86(24):17696-17709.
[26] Liang C J, Huang C F, Mohanty N, et al. A rapid spectrophotometric determination of persulfate anion in ISCO [J]. Chemosphere 2008, 73(9):1540-1543.
[27] Li J, Pham A N, Dai R, et al. Recent advances in Cu-Fenton systems for the treatment of industrial waste: Role of Cu complexes and Cu composites [J]. Journal of Hazardous Materials. 2020,392,122261.
[28] Hu H, Miao K, Luo X, et al. Efficient Fenton-like treatment of high-concentration chlorophenol wastewater catalysed by Cu-doped SBA-15mesoporous silica [J]. Journal of Cleaner Production, 2021, 318,128632.
[29] Zu D, Song H R, Li C, et al. Understanding the self-catalyzed decomplexation mechanism of Cu-EDTA in Ti₃C₂T_x MXene/ peroxymonosulfate process [J]. Applied Catalysis B: Environment. 2022,306,121131.
[30] 王义.UV/氯高级氧化体系去除Cu(II)络合物的效能与机理[D]. 温州:温州大学, 2020. Wang Y, Efficiency and Mechanism of Removal of Cu (II)-organic Complexes by UV/Chlorine [D]. Wenzhou: Wenzhou University, 2020.
[31] W D, Dong Z L, Lim T T, et al. Generation of sulfate radical through heterogeneous catalysis for organic contaminants removal: Current development, challenges and prospects [J]. Applied Catalysis B: Environment, 2016,194:169-201.
[32] Lu Y, Li D, Liu F, et al. Characterizing the chemical structure of Ti₃C₂Tx MXene by angle-resolved XPS combined with argon ion etching [J]. Materials (Basel), 2022,15(1),307.
[33] Han X, An L, Hu Y, et al. Ti₃C₂MXene-derived carbon-doped TiO₂ coupled with g-C₃N₄ as the visible-light photocatalysts for photocatalytic H₂ generation [J]. Applied Catalysis B: Environment, 2020,265,118539.
[34] Mao S, Sun X, Qi H, et al. Cu₂O nanoparticles anchored on 3D bifunctional CNTs/copper foam cathode for electrocatalytic degradation of sulfamethoxazole over a broad pH range [J]. Total Environment, 2021,793,148492.
[35] Chen Q, An X, Liu Q, et al. Boosting electrochemical nitrite-ammonia conversion properties by a Cu foam@Cu₂O catalyst [J]. Chemical Communications, 2022,58(4):517-520.
[36] Ivanova T M, Maslakov K I, Sidorov A A, et al. XPS detection of unusual Cu (II) to Cu(I) transition on the surface of complexes with redox-active ligands [J]. Journal Of Electron Spectroscopy and Related Phenomena, 2020,238,146878.
[37] Liu W, An Z, Qin L, et al. Construction of a novel ion imprinted film to remove low concentration Cu²⁺ from aqueous solution [J]. Chemical Engineering Journal. 2021,411,128477.
[38] Feng Y, Ying G G, Yang Z Q, et al. Sulfate radical-induced destruction of emerging contaminants using traces of cobalt ions as catalysts [J]. Chemosphere, 2020,256,127061.
[39] Kohantorabi M, Moussavi G, Giannakis S. A review of the innovations in metal- and carbon-based catalysts explored for heterogeneous peroxymonosulfate (PMS) activation, with focus on radical vs. non-radical degradation pathways of organic contaminants [J]. Chemical Engineering Journal, 2021,411,127957.
[40] Zhou Y, Jiang J, Gao Y, et al. Activation of peroxymonosulfate by benzoquinone: A novel nonradical oxidation process [J]. Environmental Science & Technology, 2015,49(21):12941-12950.
[41] Guo Q, Wang Z, Pang S Y, et al. Kinetic and mechanistic insights into the oxidative transformation of atrazine by aqueous Fe(IV): Comparison with hydroxyl and sulfate radicals [J]. ACS ES&T Engineering, 2023,3(9):1402-1412,1402.
[42] Cai J J, Zhou M H, Zhang Q Z, et al. The radical and non-radical oxidation mechanism of electrochemically activated persulfate process on different cathodes in divided and undivided cell [J]. Journal Of Hazardous Materials, 2021,416,125804.
[43] Wang Q, Zeng H, Liang Y, et al. Degradation of bisphenol AF in water by periodate activation with FeS (mackinawite) and the role of sulfur species in the generation of sulfate radicals [J]. Chemical Engineering Journal, 2021,407,126738.
[44] Wang J, Wang S. Reactive species in advanced oxidation processes: Formation, identification and reaction mechanism [J]. Chemical Engineering Journal, 2020,401,126158.
[45] Fang J Y, Fu Y, Shang C. The roles of reactive species in micropollutant degradation in the UV/free chlorine system [J]. Environmental Science & Technology, 2014,48(3):1859-1868.
[46] Kim C, Thao T T, Kim J H, et al. Effects of the formation of reactive chlorine species on oxidation process using persulfate and nano zero-valent iron [J]. Chemosphere, 2020,250,126266.
[47] Zhuan R, Wang J. Degradation of diclofenac in aqueous solution by ionizing radiation in the presence of humic acid. Separation and Purification Technology [J]. 2020,234,116079.
[48] Yang B, Cheng X, Zhang Y, et al. Staged assessment for the involving mechanism of humic acid on enhancing water decontamination using H₂O₂-Fe (III) process [J]. Journal of Hazardous Materials, 2021,407, 124853.
[49] Yu C, Zhang Y, Lu Y, et al. Mechanistic insight into humic acid- enhanced hydroxyl radical production from Fe (II)-bearing clay mineral oxygenation [J]. Environmental Science & Technology, 2021,55(19):13366-13375.