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Progress in Chemistry 2022, Vol. 34 Issue (5): 1017-1025 DOI: 10.7536/PC210918 Previous Articles   Next Articles

• Review •

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: Revised: Online: Published:
  • 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)
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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
Fig. 1 Topological structure of 2D and 3D COFs materials[37]. Copyright 2017, AAAS
Fig. 2 Functionalized synthesis methods for COFs materials[69⇓⇓⇓~73]
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
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
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
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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