选择性离子吸附原理与材料制备

doi:10.7536/PC221005

• 综述 •

选择性离子吸附原理与材料制备

王芷铉, 郑少奎^*()

北京师范大学环境学院北京 100875

收稿日期:2022-10-14 修回日期:2023-03-20 出版日期:2023-05-24 发布日期:2023-04-30

作者简介:

郑少奎北京师范大学教授,博士生导师,主要从事微污染水/废水处理新技术研发工作。研发出以节能降耗为特征的微好氧活性污泥UMSB工艺;基于物化方法的微污染水(地下水、污水处理厂尾水)深度净化与再生新工艺与设备。

基金资助:
国家自然科学基金项目(22176015)

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Selective Ionic Removal Strategy and Adsorbent Preparation

Zhixuan Wang, Shaokui Zheng()

School of Environment, Beijing Normal University,Beijing 100875, China

Received:2022-10-14 Revised:2023-03-20 Online:2023-05-24 Published:2023-04-30
Contact: * e-mail: zsk@bnu.edu.cn
Supported by:
National Natural Science Foundation of China(22176015)

制备特定无机阴、阳离子的选择性吸附材料有利于保障饮用水安全、控制外排污水生态风险、保障地表水环境质量,具有非常广泛的市场需求和应用前景。选择性离子吸附材料研发始于20世纪60年代,经过60年的高速发展,选择性离子吸附材料领域目前依旧保持了极高的研究热度和研究水平。本文概述了选择性离子吸附材料的研发历史、现状和主要研究方向,重点总结了四种选择性离子吸附原理(即分子印迹技术原理、软硬酸碱理论、非静电作用原理和竞争离子自我抑制原理)和它们的研究历史、选择性离子吸附材料制备与应用情况,展望了未来的研究方向,这些信息的整理归纳将为未来的选择性离子吸附材料研发、水中特定离子浓度控制提供重要的借鉴。

关键词： 选择性离子吸附, 原理, 水处理, 吸附剂, 研究进展

The selective ionic removal from water or wastewater by newly-developed adsorbents has been intensely investigated around the world since 1960s. These selective ionic adsorbents were used to control the concentrations of specific ions in drinking water or wastewater in the presence of plentiful coexisting ions to prepare quality drinking water or avoid ecological hazards in natural waterbodies due to wastewater discharge. Due to remarkable market demands and wide application prospects, this topic still generates numerous amazing findings in terms of international publications in recent decade. Besides the history, the present status and the research bias, this paper lays particular emphasis on the four selective ionic removal strategies involved in previous studies (i.e., the molecular imprinting technology, the soft and hard acid base theory, the non-electrostatic interaction theory, and the self-inhibition theory of competitive ions), including their mechanisms, histories, and adsorbent preparations and applications. Finally, this review also prospects the future research directions. This review provides overall information for the further development of selective ionic adsorbents for water or wastewater treatment.

Contents

1 Introduction

2 Selective ion adsorption materials based on molecular imprinting technology

2.1 Principles and development history of molecular imprinting technology

2.2 Preparation of molecularly imprinted materials and selective ion adsorption

3 Selective ion adsorption materials based on hard and soft acid base theory

3.1 The development history of acid-base theory

3.2 Preparation of hard and soft acid base materials and selective ion adsorption

4 Selective anion adsorption materials based on non-electrostatic interaction

4.1 Selective ion adsorption based on hydrophilicity and hydrophobicity

4.2 Selective ion adsorption based on hydrogen bonding

5 Selective ion adsorption of standard resin based on competitive ion self-inhibition mechanism

6 Conclusion and outlook

Key words: selective ionic removal, strategy, water treatment, adsorbent

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图1 2018—2022年(8月)选择性离子吸附材料领域国际论文发表情况

Fig. 1 Number of international publications on selective ionic materials during 2018—2022 (August)

图2 2018—2022年(8月)选择性离子吸附材料领域国际论文中的目标离子类型

Fig. 2 Target ionic types investigated in international papers on selective ionic materials during 2018—2022 (August)

图3 印迹聚合物的原理[66]

Fig. 3 Principles of imprinted polymers[66]

图4 GO-IIP的XPS图谱:(a) 吸附Pb(Ⅱ)前后的调查图谱;(b) Pb(Ⅱ)吸附后的Pb 4f光谱;吸附前(c)和吸附后(d)的N 1s谱;吸附前(e)和吸附后(f)的O1 s光谱[86]

Fig. 4 XPS spectra of GO-IIP: (a) survey spectra before and after Pb(Ⅱ) adsorption; (b) Pb 4f spectrum after Pb(Ⅱ) adsorption; N 1 s spectra before adsorption (c) and after adsorption (d); O1 s spectra before adsorption (e) and after adsorption (f)[86]

表1 部分路易斯碱的绝对硬度[89]

Table 1 Absolute hardness of some Lewis bases[89]

Base	Absolute hardness ( $η B b$ )	Base	Absolute hardness ( $η B b$ )
F^-	7.0	CN^-	5.3
Cl^-	4.7	SH^-	4.1
Br^-	4.2	ClO^-	4.5
I^-	3.7	CO^-	6.0
$NH 2 -$	5.3	H₂O	7.0
OH^-	5.6	H₂S	5.3
NO^-	4.5	NH₃	6.9

表1 部分路易斯碱的绝对硬度[89]

Table 1 Absolute hardness of some Lewis bases[89]

Base	Absolute hardness ( $η B b$ )	Base	Absolute hardness ( $η B b$ )
F^-	7.0	CN^-	5.3
Cl^-	4.7	SH^-	4.1
Br^-	4.2	ClO^-	4.5
I^-	3.7	CO^-	6.0
$NH 2 -$	5.3	H₂O	7.0
OH^-	5.6	H₂S	5.3
NO^-	4.5	NH₃	6.9

表2 部分路易斯酸的绝对硬度[89]

Table 2 Absolute hardness of some Lewis acids[89]

Acid	Absolute hardness ( $η A b$ )	Acid	Absolute hardness ( $η B b$ )
H⁺	∞	Zn²⁺	10.8
Li⁺	35.1	Hg²⁺	7.7
Na⁺	21.1	Pb²⁺	8.5
Rb⁺	11.7	Ba²⁺	12.8
Cu⁺	6.3	Pd²⁺	6.8
Ag⁺	6.9	Cd²⁺	10.3
Au⁺	5.7	Al³⁺	45.8
Mg²⁺	32.5	Sc³⁺	24.6
Ca²⁺	19.7	Fe³⁺	13.1
Ti²⁺	7.0	La³⁺	15.4
Mn²⁺	9.3	I₂	3.4
Fe²⁺	7.3	Cl₂	4.5
Ni²⁺	8.5	CO₂	6.9
Cu²⁺	8.3	SO₂	5.6

表2 部分路易斯酸的绝对硬度[89]

Table 2 Absolute hardness of some Lewis acids[89]

Acid	Absolute hardness ( $η A b$ )	Acid	Absolute hardness ( $η B b$ )
H⁺	∞	Zn²⁺	10.8
Li⁺	35.1	Hg²⁺	7.7
Na⁺	21.1	Pb²⁺	8.5
Rb⁺	11.7	Ba²⁺	12.8
Cu⁺	6.3	Pd²⁺	6.8
Ag⁺	6.9	Cd²⁺	10.3
Au⁺	5.7	Al³⁺	45.8
Mg²⁺	32.5	Sc³⁺	24.6
Ca²⁺	19.7	Fe³⁺	13.1
Ti²⁺	7.0	La³⁺	15.4
Mn²⁺	9.3	I₂	3.4
Fe²⁺	7.3	Cl₂	4.5
Ni²⁺	8.5	CO₂	6.9
Cu²⁺	8.3	SO₂	5.6

表3 常见的软硬酸碱[130]

Table 3 Typical soft and hard acids and bases[130]

Type	Ions
Soft acid	Pd²⁺, Pt²⁺, Pt⁴⁺, Cu⁺, Ag⁺, Cd²⁺, Hg²⁺, Br₂, I₂
Borderline acid	Fe²⁺, Co²⁺, Ni²⁺, Cu²⁺, Zn²⁺, Ru³⁺, Sn²⁺, Pb²⁺, Sb²⁺
Hard acid	H⁺, Li⁺, Na⁺, K⁺, Mg²⁺, Sr²⁺, Sc³⁺, La³⁺, Ce⁴⁺, Zr⁴⁺
Soft base	H^-, C₂H₄, C₆H₆, CN^-, SCN^-, R₃P
Borderline base	C₆H₅NH₂, C₅H₅N, $NO 2 -$ , $SO 3 2 -$ , Br^-
Hard base	NH₃, N₂H₄, OH^-, $PO 3 3 -$ , $CO 3 2 -$ , $NO 3 -$ , $PO 4 3 -$ , $SO 4 2 -$ , $ClO 4 -$ , F^-

表3 常见的软硬酸碱[130]

Table 3 Typical soft and hard acids and bases[130]

Type	Ions
Soft acid	Pd²⁺, Pt²⁺, Pt⁴⁺, Cu⁺, Ag⁺, Cd²⁺, Hg²⁺, Br₂, I₂
Borderline acid	Fe²⁺, Co²⁺, Ni²⁺, Cu²⁺, Zn²⁺, Ru³⁺, Sn²⁺, Pb²⁺, Sb²⁺
Hard acid	H⁺, Li⁺, Na⁺, K⁺, Mg²⁺, Sr²⁺, Sc³⁺, La³⁺, Ce⁴⁺, Zr⁴⁺
Soft base	H^-, C₂H₄, C₆H₆, CN^-, SCN^-, R₃P
Borderline base	C₆H₅NH₂, C₅H₅N, $NO 2 -$ , $SO 3 2 -$ , Br^-
Hard base	NH₃, N₂H₄, OH^-, $PO 3 3 -$ , $CO 3 2 -$ , $NO 3 -$ , $PO 4 3 -$ , $SO 4 2 -$ , $ClO 4 -$ , F^-

图5 含巯基冷冻凝胶吸附去除水中Hg2+[96]

Fig. 5 Removal of Hg2+ from water by sulfhydryl frozen gel[96]

图6 Hg2+吸附前后的(a) FTIR, (b) XPS, (c) Hg 4f和(d) 吸附剂的S 2p光谱[132]

Fig. 6 (a) FTIR, (b) XPS, (c) Hg 4f and (d) S 2p spectra of adsorbent before and after Hg2+adsorption[132]

表4 常见阴离子的水合能(Δh H I ∞)[146]

Table 4 Hydration energy of typical anions[146]

Ion	-Δ_h $H I ∞$ / kJ·mol^-1	Ion	-Δ_h $H I ∞$ / kJ·mol^-1
F^-	510	$ClO 4 -$	246
Cl^-	367	$BrO 3 -$	376
Br^-	336	I $O 3 -$	450
I^-	291	$ReO 4 -$	244
CN^-	346	$HCO 3 -$	384
SCN^-	311	$\mathrm{H}_{2}\mathrm{PO}^{-}_{4}$	522
$NO 3 -$	312	$CO 3 2 -$	1397
$SO 4 2 -$	1035	$SeO 4 2 -$	964
$CrO 4 2 -$	1261	$PO 4 3 -$	2879

表4 常见阴离子的水合能(Δh H I ∞)[146]

Table 4 Hydration energy of typical anions[146]

Ion	-Δ_h $H I ∞$ / kJ·mol^-1	Ion	-Δ_h $H I ∞$ / kJ·mol^-1
F^-	510	$ClO 4 -$	246
Cl^-	367	$BrO 3 -$	376
Br^-	336	I $O 3 -$	450
I^-	291	$ReO 4 -$	244
CN^-	346	$HCO 3 -$	384
SCN^-	311	$\mathrm{H}_{2}\mathrm{PO}^{-}_{4}$	522
$NO 3 -$	312	$CO 3 2 -$	1397
$SO 4 2 -$	1035	$SeO 4 2 -$	964
$CrO 4 2 -$	1261	$PO 4 3 -$	2879

图7 (a) Purolite A-520E和(b) 双功能(RO-02-119)树脂珠的矿床和表面形态扫描电子显微图像[142]

Fig. 7 Scanning electron microscopic images showing the mineral deposits and surface morphology of (a) Purolite A-520E and (b) bifunctional (RO-02-119) resin beads[142]

图8 (a)吸附前后Zn2Al PMA LDHs之间XPS C 1s峰的演变,以及(b)吸附后Zn2Al-PMA LDHs和Zn2Al Cl LDHs的XPS P 2p峰的比较[149]

Fig. 8 (a) Evolution of the XPS C 1s peaks between Zn2Al-PMA-LDHs before and after adsorption and (b) comparison of the XPS P 2p peaks between Zn2Al-PMA-LDHs and Zn2Al-Cl-LDHs after adsorption[149]

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