铁酸镍基水热炭协同次氯酸根氧化去除废水中铊

林茂; 李伙生; 张高生; 张平; 龙建友; 肖唐付; 张鸿郭; 熊静芳; 陈永亨

doi:10.11949/j.issn.0438-1157.20181453

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铁酸镍基水热炭协同次氯酸根氧化去除废水中铊

能源和环境工程 | 更新时间：2026-07-24

- 铁酸镍基水热炭协同次氯酸根氧化去除废水中铊
- Removal of Tl from wastewater by nickel ferrite-based hydrothermal carbon coupled with hypochlorite oxidation
- 化工学报 2019年70卷第4期页码：1591-1604
- 作者机构：
  
  1. 广州大学化学化工学院，珠江三角洲水质安全与保护教育部重点实验室，广东广州 510006
  2. 广州大学大湾区环境研究院，广东广州 510006
  3. 广州大学环境科学与工程学院，广东广州 510006
  4. 广州大学-林雪平大学城市可持续发展研究中心，广东广州 510006
- 作者简介：
  
  林茂(1993—)，男，硕士研究生，13253420204@qq.com
  陈永亨(1954—)，男，博士，教授，chenyong_heng@163.com
- 基金信息：
  
  国家自然科学基金项目(41573119;51808144)
- DOI：10.11949/j.issn.0438-1157.20181453
  中图分类号： TQ 085⁺.41
- 收稿：2018-12-05，
  
  修回：2019-01-24，
  
  网络首发：2020-06-15，
  
  纸质出版：2019-04-12
- 稿件说明：
移动端阅览
林茂, 李伙生, 张高生, 张平, 龙建友, 肖唐付, 张鸿郭, 熊静芳, 陈永亨. 铁酸镍基水热炭协同次氯酸根氧化去除废水中铊[J]. 化工学报, 2019, 70(4): 1591-1604

LIN Mao, LI Huosheng, ZHANG Gaosheng, ZHANG Ping, LONG Jianyou, XIAO Tangfu, ZHANG Hongguo, XIONG Jingfang, CHEN Yongheng. Removal of Tl from wastewater by nickel ferrite-based hydrothermal carbon coupled with hypochlorite oxidation[J]. CIESC Journal, 2019, 70(4): 1591-1604
林茂, 李伙生, 张高生, 张平, 龙建友, 肖唐付, 张鸿郭, 熊静芳, 陈永亨. 铁酸镍基水热炭协同次氯酸根氧化去除废水中铊[J]. 化工学报, 2019, 70(4): 1591-1604 DOI： 10.11949/j.issn.0438-1157.20181453.

LIN Mao, LI Huosheng, ZHANG Gaosheng, ZHANG Ping, LONG Jianyou, XIAO Tangfu, ZHANG Hongguo, XIONG Jingfang, CHEN Yongheng. Removal of Tl from wastewater by nickel ferrite-based hydrothermal carbon coupled with hypochlorite oxidation[J]. CIESC Journal, 2019, 70(4): 1591-1604 DOI： 10.11949/j.issn.0438-1157.20181453.

摘要

以铁酸镍和葡萄糖为原料构建炭包裹的磁性水热炭（NiFe

@C）作为可重复利用的高效吸附剂，并催化次氯酸根协同氧化以去除废水中的铊。考察了初始pH、混凝pH、反应温度、共存物和氧化剂投加量等因素对除铊的影响，结合X射线粉末衍射仪（XRD）、X射线光电子能谱（XPS）和电子自旋共振光谱仪（ESR）等表征手段探究了其除铊机理。在铊初始浓度20 mg/L、初始pH 10、吸附剂投加量0.5 g/L、次氯酸钠投量10 mmol/L时，铊去除率达到99%以上。Ca

、Mg

、EDTA、DPTA抑制除铊。吸附过程更适合拟一级动力学模型，等温吸附更适用于Langmuir和Temkin方程描述，最大铊吸附量达989 mg/g。NiFe

@C对Tl(I)的去除机理主要为氧化沉淀和表面羟基络合。材料再生实验表明NiFe

@C有很好的脱附与再生能力。本研究为废水除铊提供了一定的理论和技术参考依据。

Abstract

In this study

carbon-coated magnetic hydrothermal carbon (NiFe

@C) was constructed from nickel ferrite and gl

ucose as a reusable high-efficiency adsorbent

and the hypochlorite was catalyzed by oxidation to remove strontium from wastewater. The effects of initial pH

coagulation pH

reaction temperature

co-existing substance and hypochlorite dosage on thallium removal were examined

and mechanism on thallium removal was investigated by X-ray powder diffractometry (XRD)

X-ray photoelectron spectroscopy (XPS) and electron spin resonance spectroscopy (ESR). When the initial concentration of thallium was 20 mg/L

the initial pH was 10

the adsorbent dosage was 0.5 g/L

and the sodium hypochlorite dosage was 10 mmol/L

the thallium removal efficiency reached more than 99%. Ca

EDTA

and DPTA can inhibit thallium removal. The adsorption process is more suitable for the pseudo-first order kinetic model

and isothermal adsorption is more suitable for the description of Langmuir and Temkin equation. The saturated adsorption capacity is high up to 989 mg/g. The removal mechanism of Tl(I) by NiFe

@C was mainly surface hydroxyl complexation and oxidation precipitation. Material regeneration experiments show that NiFe

@C has a good ability of desorption and regeneration. This study provides a theoretical and technical reference for thallium removal in wastewater.

关键词

Keywords

references

Belzile N , Chen Y W . Thallium in the environment: a critical review focused on natural waters, soils, sediments and airborne particles [J ] . Applied Geochemistry , 2017 , 84 : 218 - 243 .

Peter A L J , Viraraghavan T . Thallium: a review of public health and environmental concerns [J ] . Environment International , 2005 , 31 ( 4 ): 493 - 501 .

Li P , Zhang J , Wang J , et al . Heavy metal(loid) pollution in mine wastes of a Carlin-type gold mine in southwestern Guizhou, China and its environmental impacts [J ] . Chinese Journal of Geochemistry , 2015 , 34 ( 3 ): 311 - 319 .

Liu J , Luo X , Wang J , et al . Thallium contamination in arable soils and vegetables around a steel plant—a newly-found significant source of Tl pollution in South China [J ] . Environmental Pollution , 2017 , 224 : 445 - 453 .

Chen Y , Wang C , Liu J , et al . Environmental exposure and flux of thallium by industrial activities utilizing thallium-bearing pyrite [J ] . Science China Earth Sciences , 2013 , 56 ( 9 ): 1502 - 1509 .

Martin L A , Wissocq A , Benedetti M F , et al . Thallium (Tl) sorption onto illite and smectite: implications for Tl mobility in the environment [J ] . Geochimicaet Cosmochimica Acta , 2018 , 230 : 1 - 16 .

吴颖娟 , 陈永亨 , 王正辉 , 等 . 环境介质中铊的分布和运移综述 [J ] . 地球与环境 , 2001 , 29 ( 1 ): 52 - 56 .

Wu Y J , Chen Y H , Wang Z H , et al . A summary of the distribution and migration of thallium in environmental media [J ] . Geology-Geochemistry , 2001 , 29 ( 1 ): 52 - 56 .

Pu Y , Yang X , Zheng H , et al . Adsorption and desorption of thallium(Ⅰ) on multiwalled carbon nanotubes [J ] . Chemical Engineering Journal , 2013 , 219 : 403 - 410 .

Zhang G , Fan F , Li X , et al . Superior adsorption of thallium(Ⅰ) on titanium peroxide: performance and mechanism [J ] . Chemical Engineering Journal , 2018 , 331 : 471 - 479 .

Memon S Q , Memon N , Solangi A R , et al . Sawdust: a green and economical sorbent for thallium removal [J ] . Chemical Engineering Journal , 2008 , 140 ( 1/2/3 ): 235 - 240 .

邓红梅 , 王耀龙 , 吴宏海 , 等 . γ-MnO 2 对Tl(Ⅰ)的吸附性能 [J ] . 环境科学研究 , 2015 , 28 ( 1 ): 103 - 109 .

Deng H M , Wang Y L , Wu H H , et al ． Characteristics of Tl(Ⅰ) adsorption on γ-MnO 2 [J ] . Research of Environmental Sciences , 2015 , 28 ( 1 ): 103 - 109 .

黄秋安 , 邓辉辉 , 姚利兵 , 等 . 碳包覆MnFe 2 O 4 (MnFe 2 O 4 @C)纳米球的制备及其对重金属离子[Cu(Ⅱ)、Pb(Ⅱ) ] 的去除 [J ] . 广东化工 , 2017 , 44 ( 347 ): 12 - 14 .

Huang Q A , Deng H H , Yao L B , et al ． Synthesis of carbon-coated MnFe 2 O 4 nanospheres for heavy metals [copper (Ⅱ) and lead (Ⅱ) ] removal [J ] . Guangdong Chemical Industry , 2017 , 44 ( 347 ): 12 - 14 .

Paulraj A , Kiros Y , Göthelid M , et al . NiFeO x as a bifunctional electrocatalyst for oxygen reduction (OR) and evolution (OE) reaction in alkaline media [J ] . Catalysts , 2018 , 8 ( 8 ): 328 .

Naushad M , Ahamad T , Al-Maswari B M , et al . Nickel ferrite bearing nitrogen-doped mesoporous carbon as efficient adsorbent for the removal of highly toxic metal ion from aqueous medium [J ] . Chem. Eng. J. , 2017 , 330 : 1351 - 1360 .

许杰龙任随周 , 张国霞 , 等 . pH及浓度对次氯酸钠除藻效果的影响 [J ] . 安徽农业科学 , 2011 , 39 ( 17 ): 10353 - 10355 .

Xu J L , Ren S Z , Zhang G X , et al . Study on algae removal effect of sodium hypochlorite under different concentration and pH value [J ] . Journal of Anhui Agricultural Sciences , 2011 , 39 ( 17 ): 10353 - 10355 .

Wang T , Jiang Z , An T , et al . Enhanced visible-light-driven photocatalytic bacterial inactivation by ultrathin carbon-coated magnetic cobalt ferrite nanoparticles [J ] . Environmental Science & Technology , 2018 , 52 ( 8 ): 4774 - 4784 .

Li X , Tang D , Tang F , et al . Preparation, characterization and photocatalytic activity of visible-light-driven plasmonic Ag/AgBr/ZnFe 2 O 4 nanocomposites [J ] . Materials Research Bulletin , 2014 , 56 : 125 - 133 .

Villar Da Gama B M , Elisandra Do Nascimento G , Silva Sales D C , et al . Mono and binary component adsorption of phenol and cadmium using adsorbent derived from peanut shells [J ] . Journal of Cleaner Production , 2018 , 201 : 219 - 228 .

李冬 . 基于碳量子点荧光探针的Cr(Ⅵ)定量测定方法研究 [D ] . 重庆 : 重庆大学 , 2017 .

Li D . Study on the quantitative determination of Cr(Ⅵ) based on carbon quantum dots as fluorescence probes [D ] . Chongqing : Chongqing University , 2017 .

Wang Y , Zhang W , Luo C , et al . Synthesis, characterization and enhanced electromagnetic properties of NiFe 2 O 4 @SiO 2 -decorated reduced graphene oxide nanosheets [J ] . Ceramics International , 2016 , 42 ( 15 ): 17374 - 17381 .

Goudarzi M , Salavati-Niasari M , Motaghedifard M , et al . Semiconductive Tl 2 O 3 nanoparticles: facile synthesis in liquid phase, characterizatio n and its applications as photocatalytic substrate and electrochemical sensor [J ] . Journal of Molecular Liquids , 2016 , 219 : 720 - 727 .

Hu Z , Shen Z , Yu J C . Converting carbohydrates to carbon-based photocatalysts for environmental treatment [J ] . Environmental Science & Technology , 2017 , 51 ( 12 ): 7076 - 7083 .

Li H J , Zhou X D , Di Y H , et al . Effect of Si-ATP/CTAB ratio on crystal morphology, pore structure and adsorption performance of hierarchical (H) ZSM-11 zeolite [J ] . Microporous and Mesoporous Materials , 2018 , 271 : 146 - 155 .

Li H , Li X , Xiao T , et al . Efficient removal of thallium(Ⅰ) from wastewater using flower-like manganese dioxide coated magnetic pyrite cinder [J ] . Chemical Engineering Journal , 2018 , 353 : 867 - 877 .

Zhao R , Li X , Sun B , et al . Preparation of phosphorylated polyacrylonitrile-based nanofiber mat and its application for heavy metal ion removal [J ] . Chemical Engineering Journal , 2015 , 268 : 290 - 299 .

黎秀菀 , 李伙生 , 张平 , 等 . MnO 2 @矿渣去除废水中的铊 [J ] . 环境工程学报 , 2018 , 12 ( 3 ): 720 - 730 .

Li X W , Li H S , Zhang P , et al . Removal of thallium from wastewater using MnO 2 @slag [J ] . Chinese Journal of Environmental Engineering , 2018 , 12 ( 3 ): 720 - 730 .

Biela R , Kučera T . Efficacy of sorption materials for nickel, iron and manganese removal from water [J ] . Procedia Engineering , 2016 , 162 : 56 - 63 .

Hashmi M S J , Rashid A , Ayaz A A , et al . Indirect determination of hypochlorite and hypobromite by thallium [J ] . Analytical Chemistry , 1966 , 38 ( 3 ): 507 - 508 .

Dash H R , Mangwani N , Das S . Characterization and potential application in mercury bioremediation of highly mercury-resistant marine bacterium Bacillus thuringiensis PW-05 [J ] . Environmental Science and Pollution Research , 2014 , 21 ( 4 ): 2642 - 2653 .

Zhi S , Tian L , Li N , et al . A novel system of MnO 2 -mullite-cordierite composite particle with NaClO for Methylene blue decolorization [J ] . Journal of Environmental Management , 2018 , 213 : 392 - 399 .

Kim K W , Lee E H , Chung D Y , et al . Manufacture characteristics of metal oxide–hydroxides for the catalytic decomposition of a sodium hypochlorite solution [J ] . Chemical Engineering Journal , 2012, 200 / 201 / 202 : 52 - 58 .

Huangfu X , Jiang J , Lu X , et al . Adsorption and oxidation of thallium(Ⅰ) by a nanosized manganese dioxide [J ] . Water , Air , & Soil Pollution , 2015 , 226 ( 1 ): 2272 .

Carlos E , Estrela C R A , Luis B E , et al . Mechanism of action of sodium hypochlorite [J ] . Braz. Dent. J. , 2002 , 13 ( 2 ): 113 - 117 .

Zhao Y , Qiu W , Yang C , et al . Removal of arsenic from flue gas by using NaClO solution [J ] . Chemical Engineering Journal , 2017 , 309 : 1 - 6 .

Yang S , Han Z , Pan X , et al . Nitrogen oxide removal from simulated flue gas by UV-irradiated electrolyzed seawater: efficiency optimization and pH-dependent mechanisms [J ] . Chemical Engineering Journal , 2018 , 354 : 653 - 662 .

Li K , Li H , Xiao T , et al . Removal of thallium from wastewater by a combination of persulfate oxidation and iron coagulation [J ] . Process Safety and Environmental Protection , 2018 , 119 : 340 - 349 .

Li H , Li X , Chen Y , et al . Removal and recovery of thallium from aqueous solutions via a magnetite-mediated reversible adsorption-desorption process [J ] . Journal of Cleaner Production , 2018 , 199 : 705 - 715 .

Li H , Chen Y , Long J , et al . Removal of thallium from aqueous solutions using Fe-Mn binary oxides [J ] . Journal of Hazardous Materials , 2017 , 338 : 296 - 305 .

王建伟 , 孙力平 , 员建 , 等 . 腐殖酸钠对钙、镁离子吸附效果的研究 [J ] . 环境科学与管理 , 2008 , 33 ( 12 ): 37 - 40 .

Wang J W , Sun L P , Yuan J , et al . Study on adsorption effect of Ca 2+ ＆Mg 2+ ion with sodium humic acid [J ] . Environmental Science and Management , 2018 , 33 ( 12 ): 37 - 40 .

Dadfarnia S , Assadollahi T , Haji Shabani A M . Speciation and determination of thallium by on-line microcolumn separation/preconcentration by flow injection-flame atomic absorption spectrometry using immobilized oxine as sorbent [J ] . Journal of Hazardous Materials , 2007 , 148 ( 1/2 ): 446 - 452 .

Li N , Tian Y , Zhao J , et al . Ultrafast selective capture of phosphorus from sewage by 3D Fe 3 O 4 @ZnO via weak magnetic field enhanced adsorption [J ] . Chemical Engineering Journal , 2018 , 341 : 289 - 297 .

Miyaji A , Kohno M , Inoue Y , et al . Hydroxyl radical generation by dissociation of water molecules during 1.65 MHz frequency ultrasound irradiation under aerobic conditions [J ] . Biochem. Biophys. Res. Commun. , 2017 , 483 ( 1 ): 178 - 182 .

Zhang H , Liu J , Ou C , et al . Reuse of Fenton sludge as an iron source for NiFe 2 O 4 synthesis and its application in the Fenton-based process [J ] . Journal of Environmental Sciences , 2017 , 53 : 1 - 8 .

Casella I G , Spera R . Electrochemical deposition of nickel and nickel–thallium composite oxides films from EDTA alkaline solutions [J ] . Journal of Electroanalytical Chemistry , 2005 , 578 ( 1 ): 55 - 62 .

Wang M , Xia Y , Qiu J , et al . Carbon quantum dots embedded mesoporous silica for rapid fluorescent detection of acidic gas [J ] . Spectrochimica Acta Part A , Molecular and Biomolecular Spectroscopy , 2019 , 206 : 170 - 176 .

Hao A , Ismail M , He S , et al . Improved unipolar resistive switching characteristics of Au-doped nickel ferrite magnetic thin films for nonvolatile memory applications [J ] . Journal of Alloys and Compounds , 2018 , 732 : 573 - 584 .

Singh P , Rana P J S , Mukherjee R , et al . A step towards environmental benign Mg/Pb based binary metal mixed halide perovskite material [J ] . Solar Energy , 2018 , 170 : 769 - 779 .

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