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説明:

Covalent organic frameworks (COFs) are promising high-performance capacitive deionization (CDI) materials. Strategies to optimize CDI performance of COFs focus largely on hybridization with conductive substrates, to improve their their intrinsically poor conductivity. A new structure-function relationship between COFs and their substrates is proposed here based on substrate-induced surface curvature. Graphene (zero-curvature) and carbon nanotubes (CNT, curved) are selected as COF growthsubstrates to assess the effect of curvature engineering effect on CDI performance of TpPa-SO3H-COF. Ultrahigh ion (Na+) adsorption capacity (58.74 mg g−1) is achieved by CNT-COF hybrid (cf. compared to graphene-COF hybrid 34.20 mg g−1), demonstrating the significance of curvature engineering. Notably, the corresponding salt (NaCl) adsorption capacity of CNT-COF hybrid reaches 149.25 mg g−1 in 1000 ppm at 1.2 V, representing state-of-the-art CDI performance, and the highest value among organic CDI electrodes. X-ray photoelectron spectroscopy and theoretical calculations subsequently reveal that substrate curvature can induce local strain, which regulates charge distribution within the COF skeleton, causing a lower binding energy state for Na+ adsorption. Electrochemical quartz crystal microbalance measurements revealed faster Na+ adsorption kinetics of CNT-COF due to regulated charge distribution within COF skeleton induced by substrate curvature. This work gives new insight into design of COF materials based on curvature engineering.

権利情報:

• Creative Commons BY Attribution 4.0 International
  

キーワード: Capacitive deionization, Covalent organic frameworks (COFs), Curvature engineering, regulation of charge distribution

刊行年月日: 2024-09-16

出版者: Wiley

掲載誌:

• Advanced Functional Materials (ISSN: 1616301X) vol. 34 issue. 45

研究助成金:

• Japan Science and Technology Agency JPMJER2003 (ERATO Project)
• Australian Laureate Fellowship Fund FL230100095

原稿種別: 出版者版 (Version of record)

MDR DOI:

公開URL: https://doi.org/10.1002/adfm.202407479

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更新時刻: 2024-12-04 14:52:44 +0900

MDRでの公開時刻: 2024-12-04 14:52:44 +0900