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双金属氮氧化物-Co单原子复合催化剂协同促进宽pH范围电催化氧气还原

赵江红 覃宇鹏 王倩靓 乔泽玉 宣佳琪 周玮

赵江红, 覃宇鹏, 王倩靓, 乔泽玉, 宣佳琪, 周玮. 双金属氮氧化物-Co单原子复合催化剂协同促进宽pH范围电催化氧气还原[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022095
引用本文: 赵江红, 覃宇鹏, 王倩靓, 乔泽玉, 宣佳琪, 周玮. 双金属氮氧化物-Co单原子复合催化剂协同促进宽pH范围电催化氧气还原[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022095
ZHAO Jiang-hong, QIN Yu-peng, WANG Qian-liang, QIAO Ze-yu, XUAN Jia-qi, ZHOU Wei. Bimetallic Oxynitride-Co Single Atom Composite Electrocatalyst Synergistically Improve Oxygen Reduction Reaction in wide pH Range[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022095
Citation: ZHAO Jiang-hong, QIN Yu-peng, WANG Qian-liang, QIAO Ze-yu, XUAN Jia-qi, ZHOU Wei. Bimetallic Oxynitride-Co Single Atom Composite Electrocatalyst Synergistically Improve Oxygen Reduction Reaction in wide pH Range[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022095

双金属氮氧化物-Co单原子复合催化剂协同促进宽pH范围电催化氧气还原

doi: 10.19906/j.cnki.JFCT.2022095
基金项目: 山西省重点研发计划项目(201903D121003);中央引导地方科技发展资金(YDZJSX2021A001);山西省科技重大专项项目(20181102019).
详细信息
    通讯作者:

    E-mail: zhaojianghong@sxu.edu.cnTel: 13834136556

  • 中图分类号: O646

Bimetallic Oxynitride-Co Single Atom Composite Electrocatalyst Synergistically Improve Oxygen Reduction Reaction in wide pH Range

Funds: Project supported by Key Research and Development Program of Shanxi Province (201903D121003), Guidance Foundation from the central government for Local Science and Technology Development (YDZJSX2021A001), Special Program for Major Science and Technology of Shanxi Province (20181102019).
  • 摘要: 缺乏高性能低成本,特别是宽pH范围响应的氧气还原电催化剂是制约低温燃料电池、金属-空气电池等多种新型能源转换技术规模化发展的关键因素之一。本论文基于传统聚合物基炭材料合成原理,通过选择合适结构的前驱体分子,在聚合过程中分子水平锚定Co原子,同时引入TiO2纳米颗粒,再经高温焙烧后制得一种双金属氮氧化物(ComTinOxNy)-Co单原子(Co-NC)复合催化剂。该催化剂在酸性(Eonset = 0.755 V vs. RHE,0.5 M H2SO4; 0.760 V vs. RHE,0.1 M HClO4)、中性(Eonset = 0.787 V vs. RHE,0.1 M PBS)、碱性(Eonset = 0.880 V vs. RHE,0.1 M KOH)电解液中的氧气还原(ORR)性能(pH = 0 ~ 13)均优于纯氮杂碳纳米管、氮杂碳纳米管负载的金属氮氧化物和Co单原子催化剂,表明ComTinOxNy与Co单原子的协同效应使得复合催化剂具有更好的ORR活性,同时复合催化剂的稳定性和选择性显著优于商品Pt/C催化剂。这为开发高性能低成本氧气还原电催化剂提供了新的思路。
  • Figure  1  (a) XRD patterns of Co-NC, Ti-NC and Co/Ti-NC-300, (b) Raman spectra of Ti-NC and Co/Ti-NC-300

    1  A schematic diagram showing synthesis process of the bimetallic oxynitride–Co single atom composite electrocatalyst

    Figure  2  (a) SEM, (b) TEM, (c) HAADF–STEM, (d) EDS–mapping, (e–g) HRTEM images of Co/Ti-NC-300 composite catalyst

    Figure  3  XPS spectra of Co/Ti-300: (a) a survey spectrum, (b) Ti 2p, (c) Co 2p and (d) N 1s high–resolution spectra; XPS spectra of Ti-NC: (b) Ti 2p and (d) N 1s high–resolution spectra

    Figure  4  In 0.1 M KOH: (a) CV and (b) LSV curves, (c) Tafel and (d) Nyquist plots (at open circuit voltage) of various catalysts

    Figure  5  (a) Polarization curves, (b) Koutecký-Levich plots, (c, d) Rotating ring-disk electrode test of Co/Ti-NC-300, (e) Methanol cross effect tests and (f) stability measurements of Co/Ti-NC-300 and Pt/C catalysts measured in 0.1 M KOH

    Figure  6  XPS spectra of Co/Ti-300 after 20 h measurement in 0.1 M KOH: (a) Ti 2p, (b) N 1s, (c) Co 2p high-resolution spectra; (d) LSV curves of Co/Ti-NC-300 measured in 0.5 M H2SO4, 0.1 M HClO4, 0.1 M PBS and 0.1 M KOH, respectively

    Table  1  Electrochemical performance parameters of different catalysts

    SampleE1/2 (mV vs. RHE)Eonset (mV vs. RHE)j0 (mA cm−2)jk (mA cm−2)
    @0.5 V vs. RHE
    b (mV dec−1)
    Co/Ti-NC-30080088035.2 × 10−915.2054
    Ti-NC707822119 × 10−98.7268
    Co -NC8088856.79 × 10−912.0148
    Pt/C8379582383 × 10−971.6159
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  • 收稿日期:  2022-11-08
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