赤泥吸附重金属离子性能及其机理研究进展

doi:10.16085/j.issn.1000-6613.2020-1352

化工进展 ›› 2021, Vol. 40 ›› Issue (6): 3455-3465.DOI: 10.16085/j.issn.1000-6613.2020-1352

赤泥吸附重金属离子性能及其机理研究进展

刘钦¹(), 周新涛¹(), 黄静², 罗中秋¹(), 邵周军¹, 王路星¹, 韦宇¹, 雒云龙¹

^1.昆明理工大学化学工程学院，云南昆明 650500
^2.西昌学院机械与电气工程学院，四川西昌 615000

收稿日期:2020-07-14 修回日期:2020-08-19 出版日期:2021-06-06 发布日期:2021-06-22
通讯作者: 周新涛,罗中秋
作者简介:刘钦（1996—），男，硕士研究生，研究方向为固体物资源化利用与安全化处理。E-mail：15827824086@163.com。
基金资助:
国家自然科学基金地区基金(21866018);昆明理工大学分析测试基金(2016T20160009);云南科技厅青年基金(2017FD093);云南教育厅资助性项目(2017ZZX147);云南省万人计划“青年拔尖人才”

Research statue on adsorption properties and mechanism of heavy metal ions using red mud

LIU Qin¹(), ZHOU Xintao¹(), HUANG Jing², LUO Zhongqiu¹(), SHAO Zhoujun¹, WANG Luxing¹, WEI Yu¹, LUO Yunlong¹

^1.Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming 650500, Yunnan, China
^2.School of Mechanical and Electrical Engineering, Xichang University, Xichang 615000, Sichuan, China

Received:2020-07-14 Revised:2020-08-19 Online:2021-06-06 Published:2021-06-22
Contact: ZHOU Xintao,LUO Zhongqiu

摘要/Abstract

摘要：

赤泥（RM）是铝土矿提取氧化铝时排放的工业废渣，对其进行改性后可作为一种低成本吸附剂有效吸附废水中的重金属离子。本文从赤泥的性质和组成进行讨论，分析赤泥吸附重金属离子的优势，总结酸改性、焙烧改性和复合改性对赤泥结构及重金属吸附性能的影响。在此基础上，阐述了赤泥吸附重金属离子的机理，列举了吸附热力学及吸附动力学模型。指出赤泥作为一种大宗工业废弃物，用作吸附剂吸附废水中的重金属离子，具有成本低、来源广泛等优点，同时可达到以废治废的目的，具有良好的应用前景。

关键词: 赤泥, 重金属离子, 改性, 吸附, 吸附机理, 废水

Abstract:

Red mud (RM) is an industrial waste residue produced in the extraction process of alumina from bauxite. Red mud could be modified as a low-cost adsorbent to efficiently adsorb heavy metal ions in wastewater. In this paper, the properties and compositions of red mud were discussed. Then, the advantages of red mud in absorbing heavy metal ions were analyzed. The effects of acid modification, roasting modification, and composite modification on the adsorption performance of red mud were summarized. Given that, the mechanisms of red mud for heavy metal ions adsorption were described. The thermodynamic and kinetic models of adsorption for heavy metals were listed. Red mud, as one of industrial wastes, has advantages for the adsorption of heavy metals from wastewater, such as low cost and ready availability, which can realize the “treatment of wastes with wastes”. In our opinion, the technology of heavy metal adsorption with red mud has a promising prospect.

Key words: red mud, heavy metal ions, modification, adsorption, adsorption mechanism, wastewater

中图分类号:

X758

刘钦, 周新涛, 黄静, 罗中秋, 邵周军, 王路星, 韦宇, 雒云龙. 赤泥吸附重金属离子性能及其机理研究进展[J]. 化工进展, 2021, 40(6): 3455-3465.

LIU Qin, ZHOU Xintao, HUANG Jing, LUO Zhongqiu, SHAO Zhoujun, WANG Luxing, WEI Yu, LUO Yunlong. Research statue on adsorption properties and mechanism of heavy metal ions using red mud[J]. Chemical Industry and Engineering Progress, 2021, 40(6): 3455-3465.

图/表 12

表1 赤泥主要化学成分（质量分数）[13-14] (%)

赤泥类型	SiO₂	CaO	Al₂O₃	Fe₂O₃	Na₂O	K₂O	TiO₂
拜耳法赤泥	3~20	2~8	10~20	30~60	2~10	—	0.1~10
烧结法赤泥	20~23	46~49	5~7	7~10	2~2.5	0.2~0.4	2.5~3
联合法赤泥	20~20.5	43~48	4.4~7.5	6.1~7.5	2.8~3	0.5~5.7	6.1~7.7

表2 赤泥矿物形式以及矿物作用离子情况[15-16]

元素	矿物	化学结构	作用离子
Fe	赤铁矿	α-Fe₂O₃	Cu²⁺、Zn²⁺、Co²⁺
	针铁矿	α-FeOOH	—
	磁铁矿	Fe₃O₄	As³⁺
	钛铁矿	FeO-TiO₂	—
	水滑石	Mg₆Al₂CO₃（OH）₁₆·4H₂O	Ni²⁺
	磁赤铁矿	γ-Fe₂O₃	—
Al	铝矾土	α-Al₂O₃·3H₂O	—
	勃姆石	γ-AlOOH	—
	三水铝石	Al（OH）₃	Cu²⁺、Zn²⁺
Ti	锐钛矿	TiO₂	—
	钙钛矿	CaTiO₃	Co²⁺
	钛铁矿	FeO-TiO₂	—
Si、Al、Na、Ca	石英	SiO₂	—
	高岭石	Al₂Si₂O₅（OH）₄	—
	埃洛石	Al₂Si₂O₅（OH）₄·H₂O	—
	方解石	CaCO₃	Cu²⁺、Zn²⁺、Cr²⁺
	方钠石	Na₄（Al₃Si₃O₁₂）Cl	Co²⁺、Cr³⁺
	霞石	Na₈（Al₆Si₆O₂₄）CO₃	—

表3 赤泥和其他吸附剂对重金属离子吸附量的比较[18-22]

吸附剂	重金属离子	吸附量/mg·g^-1	主要吸附方式	参考文献
赤泥	Cd²⁺	83.03	物理吸附、化学吸附	［18］
	Cu²⁺	21.56		［19］
	Pb²⁺	389.16		［13］
粉煤灰	Cd²⁺	0.089	化学吸附	［20］
	Cu²⁺	7		［21］
	Pb²⁺	18		［21］
黏土	Cd²⁺	39.5	物理吸附、化学吸附	［22］
	Pb²⁺	19.5	物理吸附、化学吸附	［22］

表4 不同影响因素下赤泥对重金属离子的吸附效果[18-19, 23-31]

金属离子	初始浓度 /mg?L^-1	吸附剂	吸附剂用量 /g?L^-1	吸附pH	吸附时间 /h	吸附温度 /℃	吸附量 /mg?g^-1	参考文献
Cu²⁺	100	RM	50	5.5	8	30	2.28	［23］
Cu²⁺	180	HCl-RM	4	5.5	1	23	21.56	［19］
Pb²⁺	500	HCl-RM	4	5.5	1	23	123.28	［19］
Pb²⁺	25	RM	0.5	5.5	2	25	46.68	［24］
Cd²⁺	50	RM	10	5	24	25	12.58	［25］
Cd²⁺	10	GRM	1	6.5	24	50	9	［26］
Cd²⁺	10	ARM	5	6	1	30	12.55	［27］
Cd²⁺	100	改性RM	1	4	1	30	83.03	［18］
Cd²⁺	200	RM	2	6	24	25	68	［28］
Zn²⁺	50	RM	10	5	24	25	12.05	［25］
Zn²⁺	200	RM	2	7	24	25	133	［28］
Ni²⁺	50	RM	10	5	24	25	11.06	［25］
Ni²⁺	50	HCl-RM	10	5	24	21	11.1	［29］
Co²⁺	280	RBRM	5	5	48	21	29.47	［30］
Mn²⁺	2	RM	10	6.5	1	25	0.191	［31］

图1 其他金属离子对赤泥吸附重金属离子吸附率的影响[32‐33]

图2 酸改性赤泥的SEM照片[37]

图3 H2SO4、HNO3和HCl改性赤泥流程

图4 赤泥以及不同煅烧温度下所得赤泥的XRD图[38]

图5 赤泥/有机硅烷复合材料制备

图6 赤泥吸附Cd2+的XANES光谱[44]A—CdCO3；B—CdO；C—Cd(OH)2；D—Cd(NO3)2；E—Cd(OH)Cl；F—RMnano+1mmol/L Cd；G—RMnano+6mmol/L Cd；H—RMa+1mmol/L Cd；I—RMa+6mmol/L Cd；J—RMo+1mmol/L Cd；K—RMo+6mmol/L Cd；其中：RMnano—纳米级赤泥；RMa—酸处理赤泥；RMo—初始赤泥

表5 赤泥吸附重金属离子热力学模型拟合情况[26, 30, 32, 53-57]

重金属离子	吸附剂	Langmuir等温式			Freundlich等温式			参考文献
重金属离子	吸附剂	q_m/mg?g^-1	K_L/L?mg^-1	$R 2$	$n$	K_F/L?g^-1	$R 2$	参考文献
Mn²⁺	RM	0.3348	00.007	0.5352	0.9545	57.33	0.7576	［31］
Mn²⁺	ARM700	88.36	0.071	0.945	5.56	29.77	0.820	［52］
As³⁺	RM	0.5263	0.037	0.9781	1.0710	20.48	0.9467	［31］
As³⁺	RMA	27.8	38.2		7.11	21.6		［53］
Pb²⁺	RM	6.027	2.043	0.9938	2.3469	0.1160	0.2123	［33］
Zn²⁺	ANRM	14.92	0.138	0.986	1.322	3.174	0.948	［54］
Zn²⁺	RM	12.048	0.517	0.998	4.5	4.4	0.886	［25］
Cd²⁺	IOARM	0.1163	11.3	0.957	1.464	3.681	0.994	［55］
Cd²⁺	RM	12.579	0.411	0.996	6.69	3.79	0.833	［25］
Ni²⁺	BRM0.05	11.11	0.182	0.99				［29］
Ni²⁺	BRM0.1	9.34	0.169	0.996				［29］
Ni²⁺	RM	11.062	0.167	0.997	2.76	2.08	0.878	［25］
Co²⁺	RM	9.0252	0.0184	0.9702	2.9481	0.0624	0.9335	［56］

表5 赤泥吸附重金属离子热力学模型拟合情况[26, 30, 32, 53-57]

重金属离子	吸附剂	Langmuir等温式			Freundlich等温式			参考文献
重金属离子	吸附剂	q_m/mg?g^-1	K_L/L?mg^-1	$R 2$	$n$	K_F/L?g^-1	$R 2$	参考文献
Mn²⁺	RM	0.3348	00.007	0.5352	0.9545	57.33	0.7576	［31］
Mn²⁺	ARM700	88.36	0.071	0.945	5.56	29.77	0.820	［52］
As³⁺	RM	0.5263	0.037	0.9781	1.0710	20.48	0.9467	［31］
As³⁺	RMA	27.8	38.2		7.11	21.6		［53］
Pb²⁺	RM	6.027	2.043	0.9938	2.3469	0.1160	0.2123	［33］
Zn²⁺	ANRM	14.92	0.138	0.986	1.322	3.174	0.948	［54］
Zn²⁺	RM	12.048	0.517	0.998	4.5	4.4	0.886	［25］
Cd²⁺	IOARM	0.1163	11.3	0.957	1.464	3.681	0.994	［55］
Cd²⁺	RM	12.579	0.411	0.996	6.69	3.79	0.833	［25］
Ni²⁺	BRM0.05	11.11	0.182	0.99				［29］
Ni²⁺	BRM0.1	9.34	0.169	0.996				［29］
Ni²⁺	RM	11.062	0.167	0.997	2.76	2.08	0.878	［25］
Co²⁺	RM	9.0252	0.0184	0.9702	2.9481	0.0624	0.9335	［56］

表6 赤泥吸附重金属离子动力学模型拟合情况[21, 29-30, 33, 35, 52, 54-55, 59]

重金属离子	吸附剂	准一级动力学方程			准二级动力学方程			参考文献
重金属离子		q_e/mg?g^-1	k₁/min^-1	R²	q_e/mg?g^-1	k₂/g·mg^-1·min^-1	R²	参考文献
Pb²⁺	RM		0.0822	0.882	1.9054	0.6437	0.999	［33］
Cd²⁺	RM500	16.62	0.061	0.56	18.05	0.0044	1	［35］
Cd²⁺	IOARM	0.078	0.039	0.994	0.071	5.99×10^-5	0.991	［55］
Cd²⁺	ARM	0.966	0.0795	0.905	20.6232	0.0052	0.992	［27］
Zn²⁺	ANRM	30	0.0068	0.888	25.859	3.677×10^-3	0.997	［54］
Mn²⁺	RM	17.28	0.0093	0.93	17.96	6×10^-4	0.993	［59］
Mn²⁺	RM700	78.07	0.016	0.977	87.04	2.4×10^-4	0.992	［52］
Ni²⁺	BRM0.1				6.48	0.0029	0.999	［29］
Co²⁺	RBRM				20.47	0.708	0.99	［30］
Sr²⁺	RBRM				18.22	6.044	0.99	［30］

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赤泥吸附重金属离子性能及其机理研究进展

Research statue on adsorption properties and mechanism of heavy metal ions using red mud

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