Removal of Tl from wastewater by nickel ferrite-based hydrothermal carbon coupled with hypochlorite oxidation

doi:10.11949/j.issn.0438-1157.20181453

CIESC Journal ›› 2019, Vol. 70 ›› Issue (4): 1591-1604.DOI: 10.11949/j.issn.0438-1157.20181453

• Energy and environmental engineering • Previous Articles Next Articles

Removal of Tl from wastewater by nickel ferrite-based hydrothermal carbon coupled with hypochlorite oxidation

Mao LIN¹(),Huosheng LI²,Gaosheng ZHANG²,Ping ZHANG¹,Jianyou LONG³,Tangfu XIAO³,Hongguo ZHANG^3,⁴,Jingfang XIONG³,Yongheng CHEN^1,²()

1. College of Chemistry and Chemical Engineering, Guangzhou University, Key Laboratory of Water Quality Safety and Protection of the Pearl River Delta, Ministry of Education, Guangzhou 510006, Guangdong, China
2. Environmental Research Institute of Dawan District, Guangzhou University, Guangzhou 510006, Guangdong, China
3. College of Environmental Science and Engineering, Guangzhou University, Guangzhou 510006, Guangdong, China
4. Guangzhou University-Link?ping University Urban Sustainable Development Research Center, Guangzhou 510006, Guangdong, China

Received:2018-12-05 Revised:2019-01-24 Online:2019-04-05 Published:2019-04-05
Contact: Yongheng CHEN

铁酸镍基水热炭协同次氯酸根氧化去除废水中铊

林茂¹(),李伙生²,张高生²,张平¹,龙建友³,肖唐付³,张鸿郭^3,⁴,熊静芳³,陈永亨^1,²()

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

通讯作者: 陈永亨
作者简介:<named-content content-type="corresp-name">林茂</named-content>(1993—)，男，硕士研究生，<email>13253420204@qq.com</email>|陈永亨(1954—)，男，博士，教授，<email>chenyong_heng@163.com</email>
基金资助:
国家自然科学基金项目(41573119，51808144)

Abstract

Abstract:

In this study, carbon-coated magnetic hydrothermal carbon (NiFe₂O₄@C) was constructed from nickel ferrite and glucose 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%. Ca²⁺, Mg²⁺, 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 NiFe₂O₄@C was mainly surface hydroxyl complexation and oxidation precipitation. Material regeneration experiments show that NiFe₂O₄@C has a good ability of desorption and regeneration. This study provides a theoretical and technical reference for thallium removal in wastewater.

Key words: adsorption, thallium, desorption, hydrothermal carbon, regeneration, NiFe₂O₄@C

摘要：

以铁酸镍和葡萄糖为原料构建炭包裹的磁性水热炭（NiFe₂O₄@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。Ca²⁺、Mg²⁺、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。NiFe₂O₄@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NiFe₂O₄@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。

关键词: 吸附, 铊, 脱附, 水热炭, 再生, NiFe₂O₄@C

CLC Number:

TQ 085⁺.41

Mao LIN, Huosheng LI, Gaosheng ZHANG, Ping ZHANG, Jianyou LONG, Tangfu XIAO, Hongguo ZHANG, Jingfang XIONG, Yongheng CHEN. 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.

Figures/Tables 12

Fig.1 XRD, SEM, TEM, and SAED patterns of NiFe2O4@C

Table 1 EDS-based elemental content before and after reaction

元素	质量比/%			原子量比/%
元素	吸附前	吸附后	洗脱后	吸附前	吸附后	洗脱后
C	25.80	29.40	20.73	41.85	54.27	39.85
N	1.09	0.60	0.25	1.52	0.96	0.41
O	35.87	21.86	26.19	43.81	30.29	37.80
S	0.04	0.06	0.08	0.03	0.04	0.06
Cl	0.03	0.43	1.67	0.02	0.26	1.09
Fe	24.60	21.60	35.64	8.60	8.58	14.73
Ni	12.57	10.32	15.41	4.18	3.9	6.06
Tl	0.00	15.74	0.02	0.00	1.71	0.00
sum	100.00	100.00	100.00	100.00	100.00	100.00

Fig.2 Magnetic strength, magnetic separation, FT-IR spectra and particle size distribution of NiFe2O4@C

Fig.3 Influence of pH on Tl removal, leaching of Fe and Ni, and point of zero charge analysis

Table 2 Pseudo-first and second-order kinetic model parameters

拟合模型	参数	数值
拟一级动力学模型	Q _e /(mg/g)	399.011
$y = Q e (1 - e - K 1 x)$	K ₁/h^-1	3.733
	R ²	0.981
拟二级动力学模型	Q _e/(mg/g)	400
$y = Q e x (1 / K 2 Q e + x)$	K ₂ /(g/(mg·h))	0.015
	R ²	0.953

Table 2 Pseudo-first and second-order kinetic model parameters

拟合模型	参数	数值
拟一级动力学模型	Q _e /(mg/g)	399.011
$y = Q e (1 - e - K 1 x)$	K ₁/h^-1	3.733
	R ²	0.981
拟二级动力学模型	Q _e/(mg/g)	400
$y = Q e x (1 / K 2 Q e + x)$	K ₂ /(g/(mg·h))	0.015
	R ²	0.953

Fig.4 Effect of dosage of adsorbent and sodium hypochlorite on thallium removal

Fig.5 Effect of temperature, coexisting ions and organics on Tl removal

Fig.6 Kinetic model, Tl removal within first 60 min, and isothermal adsorption

Table 3 Kinetic parameters of intra-diffusion model

K _p1/

(mg/(g·h^1/2))

C/(mg/L)

R ²

K _p2/

(mg/(g·h^1/2))

Table 4 Langmuir, Freundlich and Temkin isotherm parameters for NiFe2O4@C adsorption of Tl

Langmuir 模型

$y = Q m K X 1 + K L X$

Freundlich 模型

$q e = K F C e 1 / n$

Temkin 模型

$q e = R T b l n A C e$

Table 4 Langmuir, Freundlich and Temkin isotherm parameters for NiFe2O4@C adsorption of Tl

Langmuir 模型

$y = Q m K X 1 + K L X$

Freundlich 模型

$q e = K F C e 1 / n$

Temkin 模型

$q e = R T b l n A C e$

Q _m/(mg/g)

K _L/(L/mg)

R ²

K _F/(L/g)

R ²

A/(L/g)

b/(kJ/mol)

R ²

989

0.649

0.890

300

4.563

0.816

0.729

0.013

0.875

Fig.7 Selection of acid eluents, cyclic regeneration performance test, and leaching of nickel-iron concentration

Fig.8 Determination of free radicals(1G=10-4T)

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Removal of Tl from wastewater by nickel ferrite-based hydrothermal carbon coupled with hypochlorite oxidation

铁酸镍基水热炭协同次氯酸根氧化去除废水中铊

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