SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2024, Vol. 69 ›› Issue (5): 23-33.DOI: 10.1016/j.cjche.2024.01.022

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Enhancing capacitive deionization performance and cyclic stability of nitrogen-doped activated carbon by the electro-oxidation of anode materials

Xiaona Liu1, Baohua Zhao2, Yanyun Hu3, Luyue Huang1, Jingxiang Ma1, Shuqiao Xu1, Zhonglin Xia1, Xiaoying Ma1, Shuangchen Ma1   

  1. 1. School of Environmental Science and Engineering, North China Electric Power University, Baoding 071003, China;
    2. Huadian Zhengzhou Machinery Design and Research Institute Co., Ltd, Zhengzhou 450002, China;
    3. Huadian Inner Mongolia Energy Co., Ltd. Baotou Power Generation Branch, Baotou 014013, China
  • 收稿日期:2023-10-11 修回日期:2024-01-23 出版日期:2024-05-28 发布日期:2024-07-01
  • 通讯作者: Shuangchen Ma,E-mail:msc1225@163.com

Enhancing capacitive deionization performance and cyclic stability of nitrogen-doped activated carbon by the electro-oxidation of anode materials

Xiaona Liu1, Baohua Zhao2, Yanyun Hu3, Luyue Huang1, Jingxiang Ma1, Shuqiao Xu1, Zhonglin Xia1, Xiaoying Ma1, Shuangchen Ma1   

  1. 1. School of Environmental Science and Engineering, North China Electric Power University, Baoding 071003, China;
    2. Huadian Zhengzhou Machinery Design and Research Institute Co., Ltd, Zhengzhou 450002, China;
    3. Huadian Inner Mongolia Energy Co., Ltd. Baotou Power Generation Branch, Baotou 014013, China
  • Received:2023-10-11 Revised:2024-01-23 Online:2024-05-28 Published:2024-07-01
  • Contact: Shuangchen Ma,E-mail:msc1225@163.com

摘要: Electrode materials with high desalination capacity and long-term cyclic stability are the focus of capacitive deionization (CDI) community. Understanding the causes of performance decay in traditional carbons is crucial to design a high-performance material. Based on this, here, nitrogen-doped activated carbon (NAC) was prepared by pyrolyzing the blend of activated carbon powder (ACP) and melamine for the positive electrode of asymmetric CDI. By comparing the indicators changes such as conductivity, salt adsorption capacity, pH, and charge efficiency of the symmetrical ACP-ACP device to the asymmetric ACP-NAC device under different CDI cycles, as well as the changes of the electrochemical properties of anode and cathode materials after long-term operation, the reasons for the decline of the stability of the CDI performance were revealed. It was found that the carboxyl functional groups generated by the electro-oxidation of anode carbon materials make the anode zero-charge potential (Epzc) shift positively, which results in the uneven distribution of potential windows of CDI units and affects the adsorption capacity. Furthermore, by understanding the electron density on C atoms surrounding the N atoms, we attribute the increased cyclic stability to the enhanced negativity of the charge of carbon atoms adjacent to quaternary-N and pyridinic-oxide-N.

关键词: Anodic oxidation, Capacitive deionization, Cyclic stability, N-doping

Abstract: Electrode materials with high desalination capacity and long-term cyclic stability are the focus of capacitive deionization (CDI) community. Understanding the causes of performance decay in traditional carbons is crucial to design a high-performance material. Based on this, here, nitrogen-doped activated carbon (NAC) was prepared by pyrolyzing the blend of activated carbon powder (ACP) and melamine for the positive electrode of asymmetric CDI. By comparing the indicators changes such as conductivity, salt adsorption capacity, pH, and charge efficiency of the symmetrical ACP-ACP device to the asymmetric ACP-NAC device under different CDI cycles, as well as the changes of the electrochemical properties of anode and cathode materials after long-term operation, the reasons for the decline of the stability of the CDI performance were revealed. It was found that the carboxyl functional groups generated by the electro-oxidation of anode carbon materials make the anode zero-charge potential (Epzc) shift positively, which results in the uneven distribution of potential windows of CDI units and affects the adsorption capacity. Furthermore, by understanding the electron density on C atoms surrounding the N atoms, we attribute the increased cyclic stability to the enhanced negativity of the charge of carbon atoms adjacent to quaternary-N and pyridinic-oxide-N.

Key words: Anodic oxidation, Capacitive deionization, Cyclic stability, N-doping