3D Thioether‐Based Covalent Organic Frameworks for Selective and Efficient Mercury Removal

Zhang, Yiying; Li, Hui; Chang, Jianhong; Guan, Xinyu; Tang, Lu; Fang, Qianrong; Valtchev, Valentin; Yan, Yushan; Qiu, Shilun

doi:10.1002/smll.202006112

Cited by 41 publications

(32 citation statements)

References 77 publications

(30 reference statements)

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“…Adsorption Mechanism. The adsorption performance of TpTSC is better than other thiol 4,21,44 or thioether 40,45 functionalized adsorbents. Therefore, we believe that the coexistence of sulfur and nitrogen atoms increases the affinity and adsorption capacity for Hg(II).…”

Section: ■ Results and Discussionmentioning

confidence: 90%

Detection and Removal of Mercury Ions in Water by a Covalent Organic Framework Rich in Sulfur and Nitrogen

Tang

Qin

et al. 2022

ACS Appl. Polym. Mater.

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Hg/Hg(II) is deemed to be the most toxic heavy metal to humans. Therefore, designing suitable adsorbents to simultaneously achieve high capacity, rapid mercury adsorption, and fluorescence detection is still an important challenge in overcoming Hg2+ pollution. Here, we report a flexible alkylamine covalent organic framework (TpTSC), which has been used as an efficient adsorbent and achieves the dual-functional application of TpTSC for Hg2+, with a fluorescence detection limit of 2 ppm and simultaneously a removal capacity of 1035 mg g–1. It can remove 10 ppm mercury solution to below 2 ppb (drinking water standard) within 10 min, and the removal rate is as high as 99.98%. To a certain extent, it exceeds the recently reported thioether or thiol functionalized adsorbents. The kinetic study shows that TpTSC displays a very high K d value, with K d = 1.2 × 109 mL g–1, which has a strong affinity for mercury. In addition, TpTSC displays a good recycling capacity, with a removal rate of over 90% after five cycles. In conclusion, sulfur modification is a useful strategy for developing dual-functional COFs to simultaneously remove and detect toxic heavy metal ions.

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Section: ■ Results and Discussionmentioning

confidence: 90%

Detection and Removal of Mercury Ions in Water by a Covalent Organic Framework Rich in Sulfur and Nitrogen

Tang

Qin

et al. 2022

ACS Appl. Polym. Mater.

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“…Recently, our group designed JUC-570 and JUC-571, two 3D thioether-based COFs for mercury (Hg 2+ ) removal (Figure 5a). 55 Through the premodification of the linear building units, thioether moieties were uniformly decorated on the channel walls of the 3D dia frameworks. With a high surface area, developed channels, and exposed functional sites, these 3D materials demonstrated outstanding capacities (972 mg g −1 for JUC-570 and 970 mg g −1 for JUC-571 at pH = 5, Figure 5b), fast adsorption (distribution coefficient of 2.29 × 10 7 mL g −1 for JUC-570 and 2.07 × 10 7 mL g −1 for JUC-571), and high selectivity for mercury.…”

Section: Bottom-up Synthesis Of Functional 3d Cofs With Active Buildi...mentioning

confidence: 99%

“…In addition to functional skeletons, active pendant motifs were another important choice for bottom-up functionalization. Recently, our group designed JUC-570 and JUC-571, two 3D thioether-based COFs for mercury (Hg 2+ ) removal (Figure a) . Through the premodification of the linear building units, thioether moieties were uniformly decorated on the channel walls of the 3D dia frameworks.…”

Section: Functional Regulation Of 3d Cofsmentioning

confidence: 99%

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Functional Regulation and Stability Engineering of Three-Dimensional Covalent Organic Frameworks

et al. 2022

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Metrics & MoreArticle Recommendations CONSPECTUS: As one of the most attractive members in the porous materials family, covalent organic frameworks (COFs) have been reported thousands of times since their first discovery in 2005, covering their design, synthesis, and applications. However, an overwhelming majority of these COFs are based on two-dimensional (2D) topologies while three-dimensional (3D) COFs are numbered fewer than 100 up to date. In fact, baring enhanced specific surface area, interconnected channels, well-exposed functional moieties, and highly adjustable structures, 3D COFs are often more competitive in various application fields like adsorption, separation, chemical sensing, and heterogeneous catalysis compared with their 2D counterparts. However, significant crystallization problems and poor chemical stabilities, which might be attributed to the highly void frameworks and the absence of π−π stacking, have raised severe limitations over the research and application of 3D COFs. To solve these problems, more elaborate synthesis regulations or more moderate functionalization conditions are required. More importantly, the strategies for enhancing chemical stabilities of 3D COFs are of vital importance for their further development and practical applications.In this Account, we review the design principles, functional approaches, and stability regulation methods toward functional 3D COFs. We begin the discussion with some essential elements in the construction of 3D COF structures, including topologies, interpenetrations, linkages, and synthetic methods. After that, we focus on several strategies for the functionalization of 3D COFs, including in situ approaches (utilizing in situ generated COF linkages as the active sites), bottom-up synthesis (embedding functional moieties from predesigned building blocks), and postsynthesis modification (covalent modification or metalation of pristine frameworks). At last, we highlight some approaches toward the durable amplification of 3D COFs, which is highly important for framework functionalization and practical application. This target could be achieved through not only the introduction of some extra strengthening force, such as hydrophobic effects, coulomb repulsion, and steric hindrance effects, but also the utilization of robust linkages, which could enhance the stability from material nature. Due to their high surface area, various interpenetrated channels, multifarious functionalities, and promising stabilities, 3D COFs demonstrated excellent performance and have great potential in a wide range of application fields including adsorption and separation, heterogeneous catalysis, energy storage, and so on. Although the development of these materials has been limited by serious crystallization problems and stability restriction, great efforts have been devoted by researchers in the past decade, and a mass of strategies have been developed in synthesis control, functionalization regulation, and stability enhancement for 3D COFs. We expect 3D COFs to be practi...

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“…Earth's environment is under threat from the increasing disposal of hazardous ingredients such as heavy metals and poisonous organic and bio-organic chemicals [33][34][35][36][37][38][39]. Due to their distinct features, COFs represent themselves as viable alternative materials to address these issues [40,41]. Suitable pore designs and functionalities can render COFs as adsorbents for trapping hazardous metals, organic and bio-pollutants, and greenhouse gases [39,[42][43][44][45][46][47].…”

Section: Introductionmentioning

confidence: 99%

Structural Characteristics and Environmental Applications of Covalent Organic Frameworks

et al. 2021

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Covalent organic frameworks (COFs) are emerging crystalline polymeric materials with highly ordered intrinsic and uniform pores. Their synthesis involves reticular chemistry, which offers the freedom of choosing building precursors from a large bank with distinct geometries and functionalities. The pore sizes of COFs, as well as their geometry and functionalities, can be pre-designed, giving them an immense opportunity in various fields. In this mini-review, we will focus on the use of COFs in the removal of environmentally hazardous metal ions and chemicals through adsorption and separation. The review will introduce basic aspects of COFs and their advantages over other purification materials. Various fabrication strategies of COFs will be introduced in relation to the separation field. Finally, the challenges of COFs and their future perspectives in this field will be briefly outlined.

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3D Thioether‐Based Covalent Organic Frameworks for Selective and Efficient Mercury Removal

Cited by 41 publications

References 77 publications

Detection and Removal of Mercury Ions in Water by a Covalent Organic Framework Rich in Sulfur and Nitrogen

Detection and Removal of Mercury Ions in Water by a Covalent Organic Framework Rich in Sulfur and Nitrogen

Functional Regulation and Stability Engineering of Three-Dimensional Covalent Organic Frameworks

Structural Characteristics and Environmental Applications of Covalent Organic Frameworks

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