Emerging Covalent Organic Frameworks for Efficient Proton Conductors

Zhang, Leilang; Lyu, Bohui; Gao, Zhong; Xing, Na; Yao, Zengguang; Zhu, Shiyi; Zhang, Zhenjie; Wu, Hong; Jiang, Zhongyi

doi:10.1021/acs.iecr.3c02384

Cited by 6 publications

(1 citation statement)

References 107 publications

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“…These materials find widespread utility and are continuously evolving to meet greater challenges in industrial and sustainable applications, serving as catalysts, adsorbents, and molecular sieves. Among the most prominent examples of this category are zeolites, , metal–organic frameworks (MOFs), − and covalent organic frameworks (COFs). − The dimensions, shapes, and functional groups within their pores determine the specific chemical processes that can occur within the material. In this context, the pores within frameworks have structural and functional analogy to the active sites found in proteins, − which also contain precisely sized, functionalized pockets for binding or catalysis.…”

Section: Introductionmentioning

confidence: 99%

Pore Restructuring of Peptide Frameworks by Mutations at Distal Packing Residues

Heinz-Kunert,

Pandya,

Dang

et al. 2024

Biomacromolecules

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Porous framework materials are highly useful for catalysis, adsorption, and separations. Though they are usually made from inorganic and organic building blocks, recently, folded peptides have been utilized for constructing frameworks, opening up an enormous structure-space for exploration. These peptides assemble in a metal-free fashion using π-stacking, H-bonding, dispersion forces, and the hydrophobic effect. Manipulation of poredefining H-bonding residues is known to generate new topologies, but the impact of mutations in the hydrophobic packing region facing away from the pores is less obvious. To explore their effects, we synthesized variants of peptide frameworks with mutations in the hydrophobic packing positions and found by single-crystal X-ray crystallography (SC-XRD) that they induce significant changes to the framework pore structure. These structural changes are driven by a need to maximize van der Waals interactions of the nonpolar groups, which are achieved by various mechanisms including helix twisting, chain flipping, chain offsetting, and desymmetrization. Even subtle changes to the van der Waals interface, such as the introduction of a methyl group or isomeric replacement, result in significant pore restructuring. This study shows that the dispersion interactions upholding a peptide material are a rich area for structural engineering.

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Section: Introductionmentioning

confidence: 99%

Pore Restructuring of Peptide Frameworks by Mutations at Distal Packing Residues

Heinz-Kunert,

Pandya,

Dang

et al. 2024

Biomacromolecules

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Electrostatic Repulsion Facilitated Ion Transport in Covalent−Organic Framework Membranes

Lyu,

Jiang,

Jiang

2024

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Covalent−organic framework (COF) membranes are increasingly used for many potential applications including ion separation, fuel cells, and ion batteries. It is of central importance to fundamentally and quantitatively understand ion transport in COF membranes. In this study, a series of COF membranes is designed with different densities and arrangements of functional groups and subsequently utilize molecular simulation to provide microscopic insights into ion transport in these membranes. The membrane with a single‐sided layer exhibits the highest chloride ion (Cl−) conductivity of 77.2 mS cm−1 at 30 °C. Replacing the single‐sided layer with a double‐sided layer or changing layer arrangement leads to a decrease in Cl− conductivity up to 33% or 53%, respectively. It is revealed that the electrostatic repulsion between ions serves as a driving force to facilitate ion transport and the positions of functional groups determine the direction of electrostatic repulsion. Furthermore, the ordered pores generate concentrated ions and allow rapid ion transport. This study offers bottom‐up inspiration on the design of new COF membranes with moderate density and proper arrangement of functional groups to achieve high ion conductivity.

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Perfluoroalkyl Functionalized Superhydrophobic Covalent Organic Frameworks for Excellent Oil–Water Membrane Separation and Anhydrous Proton Conduction

Jiang,

Niu,

et al. 2024

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Rapid economic development has led to oil pollution and energy shortage. Membrane separation has attracted much attention due to its simplicity and efficiency in oil‐water‐separation. The development of membrane materials with enhanced separation properties is essential to improve the separation‐efficiency. Proton exchange membrane fuel cells (PEMFCs) are expected to replace conventional engines due to their high‐power‐conversion rates and other favorable properties. Anhydrous‐proton‐conducting materials are vital components of PEMFCs. However, developing stable proton‐conducting materials that exhibit high conductivity at varying temperatures remains challenging. Herein, two covalent organic frameworks (COFs) with long‐side‐chains are synthesized, and their corresponding COF@SSN membranes. Both membranes can effectively separate oil–water mixtures and water‐in‐oil emulsions. The TFPT‐AF membrane achieves a maximum oil‐flux of 6.05 × 105 g h−1 m−2 with an oil–water separation efficiency of above 99%, which is almost unchanged after 20 consecutive uses. COF@H3PO4 doped with different ratios of H3PO4 is prepared, the results show that the perfluorocarbon‐chain system has excellent anhydrous proton conductivity , achieving an ultra‐high proton‐conductivity of 3.98 × 10−1 S cm−1 at 125 °C. This study lays the foundation for tailor‐made‐functionalization of COF through pre‐engineering and surface‐modification, highlighting the great potential of COFs for oil‐water separation and anhydrous‐proton‐conductivity.

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Emerging Covalent Organic Frameworks for Efficient Proton Conductors

Cited by 6 publications

References 107 publications

Pore Restructuring of Peptide Frameworks by Mutations at Distal Packing Residues

Pore Restructuring of Peptide Frameworks by Mutations at Distal Packing Residues

Electrostatic Repulsion Facilitated Ion Transport in Covalent−Organic Framework Membranes

Perfluoroalkyl Functionalized Superhydrophobic Covalent Organic Frameworks for Excellent Oil–Water Membrane Separation and Anhydrous Proton Conduction

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