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化学进展 2022, Vol. 34 Issue (5): 1017-1025 DOI: 10.7536/PC210918 前一篇   后一篇

• 综述 •

共价有机框架在水中二价汞吸附去除中的应用

李诗宇1,2,3, 阴永光1,2,3, 史建波1,2,3,*(), 江桂斌1,2,3   

  1. 1.国科大杭州高等研究院环境学院 杭州 310000
    2.中国科学院生态环境研究中心环境化学与生态毒理学国家重点实验室 北京 100085
    3.中国科学院大学资源与环境学院 北京 100049
  • 收稿日期:2021-09-15 修回日期:2021-11-15 出版日期:2022-05-24 发布日期:2022-04-01
  • 通讯作者: 史建波
  • 基金资助:
    国家重点研发计划项目(2020YFA0907400); 国家自然科学基金项目(42025704); 中国科学院创新交叉团队项目(JCTD-2018-04)
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Application of Covalent Organic Frameworks in Adsorptive Removal of Divalent Mercury from Water

Shiyu Li1,2,3, Yongguang Yin1,2,3, Jianbo Shi1,2,3(), Guibin Jiang1,2,3   

  1. 1. School of Environment, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences,Hangzhou 310000, China
    2. State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences,Beijing 100085, China
    3. College of Resources and Environment, University of Chinese Academy of Sciences,Beijing 100049, China
  • Received:2021-09-15 Revised:2021-11-15 Online:2022-05-24 Published:2022-04-01
  • Contact: Jianbo Shi
  • Supported by:
    National Key Research and Development Program of China(2020YFA0907400); National Natural Science Foundation of China(42025704); CAS Interdisciplinary Innovation Team(JCTD-2018-04)

伴随现代工业的迅速发展,大量含汞化合物通过多种途径进入水环境。二价汞离子(Hg2+)是水体中汞的主要存在形态,开发先进的水体Hg2+去除技术对于降低健康风险和保障生态安全至关重要。作为有效的水处理技术之一,吸附法去除水中的Hg2+已得到了人们的关注,而寻找性能优异的吸附材料是取得突破的关键。近年来,共价有机框架(Covalent organic frameworks,COFs)凭借其高比表面积、有序的多孔结构和表面易功能化等优势,已被广泛应用于环境修复领域。本文主要综述了COFs在吸附去除水中Hg2+方面的最新进展,探讨COFs的结构设计、功能化合成、水中Hg2+吸附行为、反应机理、环境影响因素以及拓展至规模化应用的潜力,并展望该领域未来发展的新机遇。

关键词： 共价有机框架, 汞, 功能化合成, 水处理, 吸附

With the rapid development of modern industry, large amounts of mercury-containing compounds are discharged into the aqueous environment through various ways. Developing advanced technology for divalent mercury ion (Hg2+) removal from water is critical to reduce health risks and ensure ecological safety. As one of the effective water treatment technologies, the adsorptive removal of Hg2+ from aqueous solution has been concerned, and the key to make a breakthrough is to design adsorption materials with excellent performance. In recent years, covalent organic frameworks (COFs) have been widely used in the environmental remediation because of their high specific surface area, ordered porous structure and facile surface functionalization. Herein, the latest applications of COFs in adsorptive removal of Hg2+ from water are reviewed. The structure design, functionalized synthesis, Hg2+ adsorption behavior, reaction mechanism, affecting factors and potential to expand to large-scale applications of COFs are also discussed. Eventually, the future opportunities and development directions for COFs in Hg2+ removal are prospected.

Contents

1 Introduction

2 The structure and topology design of COFs

3 Functionalized synthesis of COFs

3.1 Bottom-up method

3.2 Post-synthesis modification

3.3 Physical blending method

4 Adsorption of Hg2+ from aqueous solution by COFs

4.1 Adsorption isotherm

4.2 Adsorption kinetics

4.3 Mechanism of interaction between COFs and Hg2+

4.4 Influence of coexisting metal ions and pH value

4.5 Fluorescence characteristics of COFs during adsorption

5 Conclusions and perspectives

Key words: covalent organic frameworks, mercury, functionalized synthesis, water treatment, adsorption
()
图1 二维和三维COFs材料的基本拓扑结构[37]
Fig. 1 Topological structure of 2D and 3D COFs materials[37]. Copyright 2017, AAAS
图2 功能化合成COFs材料的方法示意图[69⇓⇓⇓~73]
Fig. 2 Functionalized synthesis methods for COFs materials[69⇓⇓⇓~73]
表1 水中Hg2+的去除技术
Table 1 Removal technologies of Hg2+ from aqueous media
Techniques Advantages Disadvantages ref
Coagulation Cost effective, less equipment investment Adding amount of chemicals 3
Chemical precipitation No additional energy Requiring secondary treatment 23
Ion exchange No sludge generation Frequent regeneration and maintenance 24
Membrane separation High selectivity Easy to membrane fouling 26
Electrochemical treatment High removal efficiency High electrode cost 27
Bioremediation Less toxic by-products Management difficulties 30
Adsorption Easy operation, adsorbents have great development potential Need for desorption 25
表2 用于吸附去除水中Hg2+的COFs材料
Table 2 COFs materials for adsorptive removing Hg2+ in water
Adsorbents Adsorption capacity (mg/g) Distribution coefficients (mL/g) Adsorption equilibrium time (min) Residual Hg2+
concentration (μg/L) / adsorbent dose (g/L)		 Reactive sites Preparation strategy ref
TAPB-BMTTPA-COF 734 7.82×105 5 10/0.5 (15 min) Methylthio groups Bottom-up 56
COF-S-SH 1350 2.3×109 10 0.73/0.02 (30 min) Thiol and thioether groups Post-synthesis 57
TPB-DMTP-COF-SH 4395 3.23×109 2 19/0.5 (30 min) Thiol groups Post-synthesis 66
COF-SH 1283 — 30 <50/0.1 (30 min) Thiol groups Bottom-up 40
MSCTF-1 221 1.67×108 120 <30/1 (60 min) Thioether groups Bottom-up 77
NOP-28 658 — 10 <1/0.8 (10 min) Thioether groups Bottom-up 78
TpODH 1692 — — — Amide, amino, and
carbonyl groups		 Bottom-up 79
SCTN-1 1253 1.89×108 5 ~1/0.8 (10 min) Thioether groups Bottom-up 39
M-COF-SH 383 — 10 <200/0.5 (20 min) Thiol groups Physical blending 81
Ag NPs@COF-LZU1 113 1.67×107 10 <100/0.3 (30 min) Ag atoms Physical blending 82
表3 COFs对Hg2+吸附过程中的影响因素及再生方法
Table 3 The influencing factors and regeneration methods of COFs on Hg2+ adsorption process
Adsorbents Coexisting ions Effective pH range Regeneration method ref
TAPB-BMTTPA-COF Pb2+, Zn2+, Fe3+, Mg2+, Ca2+, K+ 0~14 6.0 M HCl 56
COF-S-SH Cu2+, Zn2+, Ca2+, Mg2+, Na+ 3~10 1,2-ethanedithiol 57
TPB-DMTP-COF-SH Sn2+, Pb2+, Cd2+, As3+, Cu2+, Ca2+, Mg2+, Zn2+, Na+ 5~12 6.0 M HCl 66
COF-SH Na+, Mg2+, Ca2+, Zn2+, Cd2+, Cu2+, Pb2+ 4~9 0.5 M HCl 40
MSCTF-1 Zn2+, Fe3+, Mg2+, K+, Ca2+, Cr3+, Mn2+, Cd2+, Cu2+, Pb2+ 2~11 6.0 M HCl 77
NOP-28 Co2+, Cu2+, Pd2+, Cd2+, Mg2+ 0~13 6.0 M HCl 78
TpODH Pb2+, Cr3+, Cd2+ — — 79
SCTN-1 K+, Na+, Zn2+, Co2+, Cd2+, Pb2+, Mg2+ 6~10 6.0 M HCl 39
M-COF-SH K+, Na+, Mg2+, Cu2+, Ca2+, Co2+, Cd2+, Pb2+, Mn2+, Ni2+, Cr3+, Al3+ 2~7 0.01 M HCl+
0.1%thiourea		 81
Ag NPs@COF-LZU1 Cd2+, Zn2+, Cu2+, Ca2+, Mg2+ 1~7 Thermal decomposition
(200 ℃)		 82
表4 用于荧光检测和去除水中Hg2+的COFs材料
Table 4 COFs materials for fluorescent detection and removal of Hg2+ in water
Adsorbents Maximum emission wavelength (nm) Absolute quantum yield (%) The detection limit (μg/L) Fluorescence quenching mechanism ref
COF-LZU8 460 3.5 25.0 Electron transfer 75
NOP-28 415 — 12 Electron transfer 78
AH-COF 603 3.8 20.0 ESIPT 86
TFPPy-CHYD 463 13.6 3.4 PET 76
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