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g-C3N4/Pb复合材料制备及其在铅炭电池负极材料中的应用

谢发之 张道德 杨少华 宋恒帅 张梦 方亮 邵永刚

谢发之, 张道德, 杨少华, 等. g-C3N4/Pb复合材料制备及其在铅炭电池负极材料中的应用[J]. 复合材料学报, 2023, 40(3): 1541-1551. doi: 10.13801/j.cnki.fhclxb.20220515.001
引用本文: 谢发之, 张道德, 杨少华, 等. g-C3N4/Pb复合材料制备及其在铅炭电池负极材料中的应用[J]. 复合材料学报, 2023, 40(3): 1541-1551. doi: 10.13801/j.cnki.fhclxb.20220515.001
XIE Fazhi, ZHANG Daode, YANG Shaohua, et al. Preparation of g-C3N4/Pb composites and application in anode materials for lead carbon batteries[J]. Acta Materiae Compositae Sinica, 2023, 40(3): 1541-1551. doi: 10.13801/j.cnki.fhclxb.20220515.001
Citation: XIE Fazhi, ZHANG Daode, YANG Shaohua, et al. Preparation of g-C3N4/Pb composites and application in anode materials for lead carbon batteries[J]. Acta Materiae Compositae Sinica, 2023, 40(3): 1541-1551. doi: 10.13801/j.cnki.fhclxb.20220515.001

g-C3N4/Pb复合材料制备及其在铅炭电池负极材料中的应用

doi: 10.13801/j.cnki.fhclxb.20220515.001
基金项目: 安徽省教育厅自然科学研究重大项目(KJ2018ZD049);国家自然科学基金(21777001;21671003)
详细信息
    通讯作者:

    谢发之,博士,教授,硕士生导师,研究方向为功能材料 E-mail: fzxie@ahjzu.edu.cn

  • 中图分类号: TQ152

Preparation of g-C3N4/Pb composites and application in anode materials for lead carbon batteries

Funds: Major Program Natural Science Foundation of the Higher Education Institutions of Anhui Province (KJ2018ZD049); National Science Foundation of China (21777001; 21671003)
  • 摘要: 为改善铅炭电池的析氢缺陷,提高电池循环使用寿命,以尿素为前驱体制备层状石墨相氮化碳(g-C3N4),并将其作为添加剂制备铅炭电池负极板,以活性炭(AC)为对照,研究了g-C3N4结构和添加量对铅炭电池电化学性能的影响。结果表明:g-C3N4的加入使析氢反应(HER)得到明显抑制,−1.5 V下1wt%g-C3N4负极板的析氢电流仅为AC负极板的5%。交流阻抗谱图显示1wt%g-C3N4和AC负极材料阻抗(Rs)为0.19868 Ω和1.749 Ω。更重要的是1wt%g-C3N4负极板比电容比1wt%AC负极板高344%。在5000 h高倍率部分荷电态(HRPSoC)下的电池循环寿命测试中,加入g-C3N4后电池寿命比加入AC提升62%。500次循环后,电池容量保持率仍有70%。g-C3N4可有效抑制析氢反应,提高比电容从而延长电池循环寿命,且成本低廉,可作为一种新的负极添加剂来改善铅炭电池性能。

     

  • 图  1  (a) 石墨相氮化碳(g-C3N4)和活性炭(AC)的XRD图谱、SEM图像;(b) g-C3N4和AC的FTIR图谱;(c) g-C3N4的吸脱附曲线与孔径分布图;(d) AC的吸脱附曲线与孔径分布图

    Figure  1.  (a) XRD patterns, SEM images of graphite phase carbon nitride (g-C3N4) and activated carbon (AC); (b) FTIR spectra of g-C3N4 and AC; (c) Adsorption and desorption curves and pore size distribution of g-C3N4; (d) AC adsorption and desorption curves and pore size distribution

    STP—Standard temperature and pressure

    图  3  (a) g-C3N4、AC的循环伏安曲线;(b) g-C3N4、AC交流阻抗图谱;(c) g-C3N4、AC的LSV曲线;(d) 不同含量的g-C3N4的LSV曲线

    Figure  3.  (a) Cyclic voltammogram of g-C3N4 and AC; (b) AC impedance patterns of g-C3N4 and AC; (c) LSV plots of g-C3N4 and AC; (d) LSV plots of g-C3N4 with different contents

    Z'—Real impedance; Z''—Imaginary impedance; HER—Hydrogen evolution reaction

    图  2  等效电路图

    Figure  2.  Analog circuit diagram

    图  4  (a) 不同添加量的g-C3N4和添加1wt%AC电池4 h充放电图;(b) 不同添加量的g-C3N4和添加1wt%AC电池的Tafer曲线;(c) 不同添加量的g-C3N4电池和AC电池的放电曲线;(d) 电池容量保持率

    Figure  4.  (a) Charge and discharge diagram for 4 h of different amounts of g-C3N4 and 1wt% AC battery; (b) Tafer curves of g-C3N4 with different supplemental levels and 1wt%AC batteries; (c) Discharge curves of g-C3N4 cells and ACcells with different concentrations; (d) Battery capacity retention chart

    HRPSoC—High-rate partial-state-of-charge; i—Polarization current density

    图  5  g-C3N4作用示意图

    Figure  5.  Schematic diagram for effect of g-C3N4

    图  6  高倍率部分荷电状态 (HRPSoC)下充放电进度示意图

    Figure  6.  Schematic diagram for charge/discharge progress under high-rate partial-state-of-charge (HRPSoC) duty

    图  7  ((a)、(b)) 加入活性炭的负极板循环前板极内部的SEM图像;((c)、(d)) 加入g-C3N4负极板循环前板极内部的SEM图像;((e)、(f)) 加入活性炭的负极板循环后板极内部的SEM图像;((g)、(h)) 加入g-C3N4负极板循环后板极内部的SEM图像

    Figure  7.  ((a), (b)) SEM images of the inside of the plate pole before the cycle of the negative plate with the addition of AC; ((c), (d)) SEM images of the inside of the plate pole before the cycle of the negative plate with the addition of g-C3N4; ((e), (f)) SEM images of the inside of the plate pole after circulation of the negative plate with the addition of AC; ((g), (h)) SEM images of the inside of the plate pole after circulation of the negative plate with the addition of g-C3N4

    图  8  (a) 添加1wt%AC和g-C3N4负极板循环后板极内部的XRD图谱;(b) 添加1wt%AC和g-C3N4负极板循环后板极PbSO4半峰宽对比图

    Figure  8.  (a) XRD patterns of the interior of the plate electrode after cycling with 1wt%AC and g-C3N4 negative plate; (b) Comparison of the half-peak width of PbSO4 at the plate electrode after cycling with 1wt%AC and g-C3N4 negative plate

    图  9  ((a)、(b)) 添加1wt%AC负极板吸脱附曲线与孔径分布图;((c)、(d)) 添加1wt%g-C3N4负极板吸脱附曲线与孔径分布图;((e)、(f)) 添加2wt%g-C3N4负极板吸脱附曲线与孔径分布图

    Figure  9.  ((a), (b)) Adsorption and desorption curves and pore size distribution of 1wt%AC negative plate; ((c), (d)) Adsorption and desorption curves of negative plate with 1wt%g-C3N4 and pore size distribution; ((e), (f)) Adsorption and desorption curves of negative plate with 2wt%g-C3N4 and pore size distribution

    表  1  Tafer曲线拟合数据值

    Table  1.   Tafer curve fitting data values

    Sampleab
    1wt%AC0.324850.29929
    0.5wt%g-C3N40.195460.17436
    1wt%g-C3N40.167000.15200
    2wt%g-C3N40.184480.16509
    3wt%g-C3N40.214370.19035
    4wt%g-C3N40.273740.25704
    Notes: a—Overpotential of the electrode at unit current density; b—Influence of polarization current density variation on electrode overpotential.
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  • 收稿日期:  2022-03-21
  • 修回日期:  2022-04-27
  • 录用日期:  2022-05-01
  • 网络出版日期:  2022-05-16
  • 刊出日期:  2023-03-15

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