Acta Chimica Sinica ›› 2023, Vol. 81 ›› Issue (8): 884-890.DOI: 10.6023/A23040132 Previous Articles     Next Articles

Special Issue: 庆祝《化学学报》创刊90周年合辑

Article

高稳定二维联咔唑sp2碳共轭共价有机框架材料用于高效电催化氧还原

刘建川, 李翠艳, 刘耀祖, 王钰杰*(), 方千荣*()   

  1. 吉林大学化学学院 无机合成与制备化学国家重点实验室 长春 130012
  • 投稿日期:2023-04-13 发布日期:2023-09-14
  • 作者简介:
    庆祝《化学学报》创刊90周年.
  • 基金资助:
    项目受国家重点研发计划(2022YFB3704900); 项目受国家重点研发计划(2021YFF0500500); 国家自然科学基金(22025504); 国家自然科学基金(21621001); 国家自然科学基金(22105082); 以及中石化石油化工科学研究院资助

Highly-Stable Two-Dimensional Bicarbazole-based sp2-Carbon-conjugated Covalent Organic Framework for Efficient Electrocatalytic Oxygen Reduction

Jianchuan Liu, Cuiyan Li, Yaozu Liu, Yujie Wang(), Qianrong Fang()   

  1. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012
  • Received:2023-04-13 Published:2023-09-14
  • Contact: *E-mail: wyujie@jlu.edu.cn; qrfang@jlu.edu.cn
  • About author:
    Dedicated to the 90th anniversary of Acta Chimica Sinica.
  • Supported by:
    National Key R&D Program of China(2022YFB3704900); National Key R&D Program of China(2021YFF0500500); National Natural Science Foundation of China(22025504); National Natural Science Foundation of China(21621001); National Natural Science Foundation of China(22105082); SINOPEC Research Institute of Petroleum Processing

With the extensive utilization of fossil fuels in industrial development, the energy crisis and environmental issues have become crucial challenges for current scientific development. The development of sustainable and clean energy is of great importance for sustainable human progress. Fuel and metal-air batteries have emerged as promising alternatives to fossil fuels, providing environmentally friendly and sustainable clean energy. Improving the efficiency of the oxygen reduction reaction (ORR) is crucial for energy generation and storage processes of batteries. Therefore, the development of efficient and stable ORR electrocatalysts is a key task to improve battery performance. Noble metal-based materials are known for their excellent ORR catalytic performance, but their high cost and instability have limited their applications. Hence, it is essential to develop low-cost, low-pollution, and high-efficiency electrocatalysts as noble metal-based alternatives. Transition-metal (TM)-based materials, metal alloys, and metal-free carbon nanomaterials have been reported as alternatives, but their properties are not as good as those of noble metal-based materials. In addition, their complex processes and difficult-to-identify active sites make it challenging to elucidate the intrinsic mechanisms. Rational design and precise synthesis of electrochemical catalysts are critical strategies. Covalent organic frameworks (COFs) have several advantages, including high crystallinity, high specific surface area, high stability, and regular pore channels. Besides, the construction of COFs has the advantages of pre-design and precise synthesis. Reasonable design and construction unit is an important strategy to realize the functional application of COFs materials. Many new products with structural characteristics have been reported since the introduction of COFs, and they have demonstrated excellent performance in several fields. In this study, we investigated the application of a highly stable sp2-carbon-linked COF (JUC-557) based on a bicarbazole building block for electrocatalytic oxygen reduction. We performed various characterizations of JUC-557, which demonstrated its high crystallinity, high specific surface area (870.64 m2/g), and regular structure. Moreover, JUC-557 exhibited excellent thermal and chemical stability. In the ORR performance test, JUC-557 showed good ORR catalytic performance, with an onset potential of 0.80 V vs. RHE, a half-wave potential of 0.68 V vs. RHE, a Tafel slope of only 62.20 mA•cm-2, and a Cdl of 5.79 mF•cm-2. Moreover, the Zn-air battery assembled with JUC-557 as an air-cathode electrode catalyst has a stable open-circuit voltage of 1.29 V and can easily light up the “COF” LED board. In conclusion, the rational construction of COFs as ORR catalysts has great potential in energy device application.

Key words: porous materials, covalent organic frameworks, electrocatalyst, oxidation reduction, metal-free catalyst