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Cl 元素掺杂 Fe-C-N 催化剂的构筑及其氧还原性能研究.

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Title: Cl 元素掺杂 Fe-C-N 催化剂的构筑及其氧还原性能研究.
Alternate Title: Construction of Cl-Doped Fe-C-N catalysts and investigation of oxygen reduction performance.
Authors: 刘新宇1 xinyu0512@mail.ustc.edu.cn, 周婉琳2, 张宇浩1, 吴久龙1, 孙海昕1, 刘庆华1, 韦世强1 sqwei@ustc.edu.cn
Source: Clean Coal Technology. May2026, Vol. 32 Issue 5, p77-89. 13p.
Subject Terms: *Oxygen reduction, *Chlorine, *Fuel cells, *Electrochemical analysis, *Metal catalysts, *Transition metal catalysts, *Iron catalysts, *Ligands (Chemistry)
Abstract (English): The purpose of this study is to solve the problem of slow kinetics and dependence on expensive platinum-based catalysts for cathode oxygen reduction reaction ( ORR ) in fuel cells. The core purpose is to develop a high-performance, low-cost non-noble metal alternative catalyst. In order to achieve this goal, a chlorine ( Cl ) doped Fe single atom catalyst ( Fe-CNCl ) was successfully prepared by introducing sodium chloride ( NaCl ) into the zeolite imidazole framework material ( ZIF-8 ) as the precursor and using the strategy of freeze-drying assistance and high-temperature pyrolysis, and systematically compared with the undoped control sample ( Fe-CN ) . The main methods used in the study include material synthesis, structural characterization and performance testing. In the synthesis, by combining the iron source with ZIF-8 and introducing NaCl as the Cl source, the target catalyst was obtained after high temperature pyrolysis and pickling. In terms of characterization, X-ray diffraction ( XRD ), scanning / transmission electron microscopy ( SEM / TEM ), X-ray photoelectron spectroscopy ( XPS ) and synchrotron radiation X-ray absorption spectroscopy ( XAS ) were used. The electrochemical performance was evaluated by rotating disk electrode (RDE) and rotating ring disk electrode ( RRDE ) in alkaline electrolyte ( 0.1 mol/L KOH ) . The research process and results show that Cl is successfully incorporated into the catalyst. XRD and electron microscopy analysis showed that the catalyst maintained the dodecahedron framework of the precursor after pyrolysis, and the iron existed in the form of atomic dispersion without forming clusters or particles. XPS and XAS analysis further revealed that the introduction of Cl formed a coordination bond ( Fe—Cl ) with Fe, breaking the high symmetry of the original Fe—N4 site and forming an asymmetric local coordination structure. Electrochemical tests show that Cl doping greatly optimizes the ORR performance. The half-wave potential ( E1/2) of Fe-CNCl is as high as 0.903 V ( vs. RHE ), which is significantly better than that of undoped Fe-CN (0.854 V) and commercial Pt / C catalyst. Its Tafel slope is lower ( 88 mV / dec ), indicating faster reaction kinetics. Through the RRDE test calculation, the electron transfer number is close to 4 ( 3.9 approximately ), and the hydrogen peroxide yield is extremely low ( 1.3% approximately), indicating that the reaction efficiently follows the four-electron path and directly generates water. In the constant potential stability test for about 70 h, the current decay rate of Fe-CNCl is only 6%, showing excellent durability far exceeding the contrast sample (Fe-CN decays by 25%, Pt / C decays by 31%). In summary, this study successfully constructed a high-performance Fe-C-N single-atom ORR catalyst through a simple Cl element doping strategy. This work not only demonstrates an efficient non-precious metal ORR catalyst, but also provides new ideas and experimental basis for the precise design of the next generation of single-atom catalysts through heteroatom axial coordination engineering. [ABSTRACT FROM AUTHOR]
Abstract (Chinese): 为解决燃料电池阴极氧还原反应 (ORR) 动力学缓慢、依赖昂贵铂基催化剂的问题, 需要开发 一种高性能、低成本的非贵金属替代催化剂. 为实现此目标, 以沸石咪唑骨架材料 (ZIF-8) 为前驱 体, 通过引入氯化钠 (NaCl) 并采用冷冻干燥辅助与高温热解的策略, 成功制备了一种氯 (Cl) 元素 掺杂的 Fe 单原子催化剂 (Fe-CNCl), 并与未掺杂的对比样 (Fe-CN) 进行系统比较. 研究采用的主 要方法包括材料合成、结构表征与性能测试. 在合成上, 通过将铁源与 ZIF-8 结合, 并引入 NaCl 作为 Cl 源, 经高温热解和酸洗后得到目标催化剂. 在表征方面, 综合运用了 X 射线衍射 (XRD) 、扫描/透 射电子显微镜 (SEM/TEM) 、 X 射线光电子能谱 (XPS) 及同步辐射 X 射线吸收谱 (XAS) 等多种技 术. 电化学性能则在碱性电解液 (0.1 mol/ L KOH) 中, 通过旋转圆盘电极 (RDE) 、旋转环盘电极 (RRDE) 等测试进行评估. 研究过程与结果表明 Cl 成功掺入催化剂. XRD 与电子显微分析表明: 催 化剂在热解后保持了前驱体的十二面体形貌框架, 且铁以原子级分散形式存在, 未形成团簇或颗粒. XPS 与 XAS 分析进一步揭示了 Cl 的引入与 Fe 形成了配位键 (Fe—Cl), 打破了原本 Fe—N4 位点的 高度对称性, 形成了不对称的局域配位结构. 电化学测试证明 Cl 掺杂极大地优化了 ORR 性能. FeCNCl 的半波电位 (E1/2) 高达 0.903 V (vs. RHE), 显著优于未掺杂的 Fe-CN (0.854 V ) 和商业 Pt/ C 催 化剂. 其 Tafel 斜率更低 (88 mV/dec), 表明反应动力学更快. 通过 RRDE 测试计算, 其电子转移数 接近 4 (约 3.9), 过氧化氢产率极低 (约 1.3% ), 说明反应高效地遵循四电子路径, 直接生成水. 在 长达约 70 h 的恒电位稳定性测试中, Fe-CNCl 的电流衰减率仅为 6%, 表现出远超对比样 (Fe-CN 衰 减 25%, Pt/ C 衰减 31% ) 的卓越耐久性. 综上所述, 通过简单的 Cl 元素掺杂策略, 成功构筑了一种高 性能 Fe- C - N 单原子 ORR 催化剂. 展示了一种高效的非贵金属 ORR 催化剂, 也为通过杂原子轴向配 位工程精准设计下一代单原子催化剂提供了新的思路与试验依据. [ABSTRACT FROM AUTHOR]
Database: Energy & Power Source
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Items – Name: Title
  Label: Title
  Group: Ti
  Data: Cl 元素掺杂 Fe-C-N 催化剂的构筑及其氧还原性能研究.
– Name: TitleAlt
  Label: Alternate Title
  Group: TiAlt
  Data: Construction of Cl-Doped Fe-C-N catalysts and investigation of oxygen reduction performance.
– Name: Author
  Label: Authors
  Group: Au
  Data: <searchLink fieldCode="AR" term="%22刘新宇%22">刘新宇</searchLink><relatesTo>1</relatesTo><i> xinyu0512@mail.ustc.edu.cn</i><br /><searchLink fieldCode="AR" term="%22周婉琳%22">周婉琳</searchLink><relatesTo>2</relatesTo><br /><searchLink fieldCode="AR" term="%22张宇浩%22">张宇浩</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22吴久龙%22">吴久龙</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22孙海昕%22">孙海昕</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22刘庆华%22">刘庆华</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22韦世强%22">韦世强</searchLink><relatesTo>1</relatesTo><i> sqwei@ustc.edu.cn</i>
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  Label: Source
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  Data: <searchLink fieldCode="JN" term="%22Clean+Coal+Technology%22">Clean Coal Technology</searchLink>. May2026, Vol. 32 Issue 5, p77-89. 13p.
– Name: Subject
  Label: Subject Terms
  Group: Su
  Data: *<searchLink fieldCode="DE" term="%22Oxygen+reduction%22">Oxygen reduction</searchLink><br />*<searchLink fieldCode="DE" term="%22Chlorine%22">Chlorine</searchLink><br />*<searchLink fieldCode="DE" term="%22Fuel+cells%22">Fuel cells</searchLink><br />*<searchLink fieldCode="DE" term="%22Electrochemical+analysis%22">Electrochemical analysis</searchLink><br />*<searchLink fieldCode="DE" term="%22Metal+catalysts%22">Metal catalysts</searchLink><br />*<searchLink fieldCode="DE" term="%22Transition+metal+catalysts%22">Transition metal catalysts</searchLink><br />*<searchLink fieldCode="DE" term="%22Iron+catalysts%22">Iron catalysts</searchLink><br />*<searchLink fieldCode="DE" term="%22Ligands+%28Chemistry%29%22">Ligands (Chemistry)</searchLink>
– Name: Abstract
  Label: Abstract (English)
  Group: Ab
  Data: The purpose of this study is to solve the problem of slow kinetics and dependence on expensive platinum-based catalysts for cathode oxygen reduction reaction ( ORR ) in fuel cells. The core purpose is to develop a high-performance, low-cost non-noble metal alternative catalyst. In order to achieve this goal, a chlorine ( Cl ) doped Fe single atom catalyst ( Fe-CNCl ) was successfully prepared by introducing sodium chloride ( NaCl ) into the zeolite imidazole framework material ( ZIF-8 ) as the precursor and using the strategy of freeze-drying assistance and high-temperature pyrolysis, and systematically compared with the undoped control sample ( Fe-CN ) . The main methods used in the study include material synthesis, structural characterization and performance testing. In the synthesis, by combining the iron source with ZIF-8 and introducing NaCl as the Cl source, the target catalyst was obtained after high temperature pyrolysis and pickling. In terms of characterization, X-ray diffraction ( XRD ), scanning / transmission electron microscopy ( SEM / TEM ), X-ray photoelectron spectroscopy ( XPS ) and synchrotron radiation X-ray absorption spectroscopy ( XAS ) were used. The electrochemical performance was evaluated by rotating disk electrode (RDE) and rotating ring disk electrode ( RRDE ) in alkaline electrolyte ( 0.1 mol/L KOH ) . The research process and results show that Cl is successfully incorporated into the catalyst. XRD and electron microscopy analysis showed that the catalyst maintained the dodecahedron framework of the precursor after pyrolysis, and the iron existed in the form of atomic dispersion without forming clusters or particles. XPS and XAS analysis further revealed that the introduction of Cl formed a coordination bond ( Fe—Cl ) with Fe, breaking the high symmetry of the original Fe—N4 site and forming an asymmetric local coordination structure. Electrochemical tests show that Cl doping greatly optimizes the ORR performance. The half-wave potential ( E1/2) of Fe-CNCl is as high as 0.903 V ( vs. RHE ), which is significantly better than that of undoped Fe-CN (0.854 V) and commercial Pt / C catalyst. Its Tafel slope is lower ( 88 mV / dec ), indicating faster reaction kinetics. Through the RRDE test calculation, the electron transfer number is close to 4 ( 3.9 approximately ), and the hydrogen peroxide yield is extremely low ( 1.3% approximately), indicating that the reaction efficiently follows the four-electron path and directly generates water. In the constant potential stability test for about 70 h, the current decay rate of Fe-CNCl is only 6%, showing excellent durability far exceeding the contrast sample (Fe-CN decays by 25%, Pt / C decays by 31%). In summary, this study successfully constructed a high-performance Fe-C-N single-atom ORR catalyst through a simple Cl element doping strategy. This work not only demonstrates an efficient non-precious metal ORR catalyst, but also provides new ideas and experimental basis for the precise design of the next generation of single-atom catalysts through heteroatom axial coordination engineering. [ABSTRACT FROM AUTHOR]
– Name: Abstract
  Label: Abstract (Chinese)
  Group: Ab
  Data: 为解决燃料电池阴极氧还原反应 (ORR) 动力学缓慢、依赖昂贵铂基催化剂的问题, 需要开发 一种高性能、低成本的非贵金属替代催化剂. 为实现此目标, 以沸石咪唑骨架材料 (ZIF-8) 为前驱 体, 通过引入氯化钠 (NaCl) 并采用冷冻干燥辅助与高温热解的策略, 成功制备了一种氯 (Cl) 元素 掺杂的 Fe 单原子催化剂 (Fe-CNCl), 并与未掺杂的对比样 (Fe-CN) 进行系统比较. 研究采用的主 要方法包括材料合成、结构表征与性能测试. 在合成上, 通过将铁源与 ZIF-8 结合, 并引入 NaCl 作为 Cl 源, 经高温热解和酸洗后得到目标催化剂. 在表征方面, 综合运用了 X 射线衍射 (XRD) 、扫描/透 射电子显微镜 (SEM/TEM) 、 X 射线光电子能谱 (XPS) 及同步辐射 X 射线吸收谱 (XAS) 等多种技 术. 电化学性能则在碱性电解液 (0.1 mol/ L KOH) 中, 通过旋转圆盘电极 (RDE) 、旋转环盘电极 (RRDE) 等测试进行评估. 研究过程与结果表明 Cl 成功掺入催化剂. XRD 与电子显微分析表明: 催 化剂在热解后保持了前驱体的十二面体形貌框架, 且铁以原子级分散形式存在, 未形成团簇或颗粒. XPS 与 XAS 分析进一步揭示了 Cl 的引入与 Fe 形成了配位键 (Fe—Cl), 打破了原本 Fe—N4 位点的 高度对称性, 形成了不对称的局域配位结构. 电化学测试证明 Cl 掺杂极大地优化了 ORR 性能. FeCNCl 的半波电位 (E1/2) 高达 0.903 V (vs. RHE), 显著优于未掺杂的 Fe-CN (0.854 V ) 和商业 Pt/ C 催 化剂. 其 Tafel 斜率更低 (88 mV/dec), 表明反应动力学更快. 通过 RRDE 测试计算, 其电子转移数 接近 4 (约 3.9), 过氧化氢产率极低 (约 1.3% ), 说明反应高效地遵循四电子路径, 直接生成水. 在 长达约 70 h 的恒电位稳定性测试中, Fe-CNCl 的电流衰减率仅为 6%, 表现出远超对比样 (Fe-CN 衰 减 25%, Pt/ C 衰减 31% ) 的卓越耐久性. 综上所述, 通过简单的 Cl 元素掺杂策略, 成功构筑了一种高 性能 Fe- C - N 单原子 ORR 催化剂. 展示了一种高效的非贵金属 ORR 催化剂, 也为通过杂原子轴向配 位工程精准设计下一代单原子催化剂提供了新的思路与试验依据. [ABSTRACT FROM AUTHOR]
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RecordInfo BibRecord:
  BibEntity:
    Identifiers:
      – Type: doi
        Value: 10.13226/j.issn.1006-6772.QQ26020401
    Languages:
      – Code: chi
        Text: Chinese
    PhysicalDescription:
      Pagination:
        PageCount: 13
        StartPage: 77
    Subjects:
      – SubjectFull: Oxygen reduction
        Type: general
      – SubjectFull: Chlorine
        Type: general
      – SubjectFull: Fuel cells
        Type: general
      – SubjectFull: Electrochemical analysis
        Type: general
      – SubjectFull: Metal catalysts
        Type: general
      – SubjectFull: Transition metal catalysts
        Type: general
      – SubjectFull: Iron catalysts
        Type: general
      – SubjectFull: Ligands (Chemistry)
        Type: general
    Titles:
      – TitleFull: Cl 元素掺杂 Fe-C-N 催化剂的构筑及其氧还原性能研究.
        Type: main
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          Name:
            NameFull: 刘新宇
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            NameFull: 周婉琳
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            NameFull: 张宇浩
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            NameFull: 吴久龙
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            NameFull: 孙海昕
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            NameFull: 刘庆华
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            NameFull: 韦世强
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            – D: 01
              M: 05
              Text: May2026
              Type: published
              Y: 2026
          Identifiers:
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              Value: 10066772
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              Value: 32
            – Type: issue
              Value: 5
          Titles:
            – TitleFull: Clean Coal Technology
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