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High Sodium Ion Storage by Multifunctional Covalent Organic Frameworks for Sustainable Sodium Batteries.

ABSTRACT: Rechargeable sodium batteries hold great promise for circumventing the increasing demand for lithium-ion batteries (LIBs) and the limited supply of lithium. However, efficient sodium ion storage remains a great impediment in this field. In this study, we report the designed synthesis of a multifunctional two-dimensional covalent organic framework featuring hexaazatrinaphthalene cores linked by imidazole moieties and demonstrate its effective performance in sodium ion storage. Benzimidazole-linked covalent organic framework (BCOF-1) was synthesized by a condensation reaction between hexaazatrinaphthalenehexamine (HATNHA) and terephthalaldehyde (TA) and exhibited a high theoretical specific capacity of 392 mA h g^-1. BCOF-1 crystallizes, forming eclipsed AA stacking and mesoporous hexagonal one-dimensional channels with high surface area (840 m² g^-1), facilitating fast ionic mobility and charge transfer and enabling high-rate capability at high current rates. BCOF-1 exhibits pseudocapacitive-like behavior with a high specific capacity of 387 mA h g^-1, an energy density of 302 W h kg^-1 at 0.1 C, and a power density of 682 W kg^-1 at 5 C. Our results demonstrate that redox-active COFs have the desired structural and electronic merits to advance the use of organic electrodes in sodium-ion storage toward sustainable and efficient batteries.

SUBMITTER: Shehab MK

PROVIDER: S-EPMC10982936 | biostudies-literature | 2024 Mar

REPOSITORIES: biostudies-literature

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High Sodium Ion Storage by Multifunctional Covalent Organic Frameworks for Sustainable Sodium Batteries.

Shehab Mohammad K MK El-Kaderi Hani M HM

ACS applied materials & interfaces 20240318 12

Rechargeable sodium batteries hold great promise for circumventing the increasing demand for lithium-ion batteries (LIBs) and the limited supply of lithium. However, efficient sodium ion storage remains a great impediment in this field. In this study, we report the designed synthesis of a multifunctional two-dimensional covalent organic framework featuring hexaazatrinaphthalene cores linked by imidazole moieties and demonstrate its effective performance in sodium ion storage. Benzimidazole-linke ...[more]

PMID: 38498858

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Project description:Covalent organic frameworks (COFs) are an emerging material family having several potential applications. Their porous framework and redox-active centers enable gas/ion adsorption, allowing them to function as safe, cheap, and tunable electrode materials in next-generation batteries, as well as CO2 adsorption materials for carbon-capture applications. Herein, we develop four polyimide COFs by combining aromatic triamines with aromatic dianhydrides and provide detailed structural and electrochemical characterization. Through density functional theory (DFT) calculations and powder X-ray diffraction, we achieve a detailed structural characterization, where DFT calculations reveal that the imide bonds prefer to form at an angle with one another, breaking the 2D symmetry, which shrinks the pore width and elongates the pore walls. The eclipsed perpendicular stacking is preferable, while sliding of the COF sheets is energetically accessible in a relatively flat energy landscape with a few metastable regions. We investigate the potential use of these COFs in CO2 adsorption and electrochemical applications. The adsorption and electrochemical properties are related to the structural and chemical characteristics of each COF, giving new insights for advanced material designs. For CO2 adsorption specifically, the two best performing COFs originated from the same triamine building block, which-in combination with force-field calculations-revealed unexpected structure-property relationships. Specific geometries provide a useful framework for Na-ion intercalation with retainable capacities and stable cycle life at a relatively high working potential (>1.5 V vs Na/Na+). Although this capacity is low compared to conventional inorganic Li-ion materials, we show as a proof of principle that these COFs are especially promising for sustainable, safe, and stable Na-aqueous batteries due to the combination of their working potentials and their insoluble nature in water.

Dataset Information

High Sodium Ion Storage by Multifunctional Covalent Organic Frameworks for Sustainable Sodium Batteries.

Publications

High Sodium Ion Storage by Multifunctional Covalent Organic Frameworks for Sustainable Sodium Batteries.

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