协同硼掺杂显著提升Co-N-C催化剂的氧还原反应活性

doi:10.61558/2993-074X.3577

电化学（中英文） ›› 2025, Vol. 31 ›› Issue (9): 2506181. doi: 10.61558/2993-074X.3577

协同硼掺杂显著提升Co-N-C催化剂的氧还原反应活性

兰畅^a^,^b^,^c^,^d, 柏景森^a^,^b^,^c^,^d, 关欣^a^,^b^,^c^,^d, 王烁^a^,^b^,^c^,^d, 张楠淑^a^,^b^,^c^,^d, 程雨晴^a^,^b^,^c^,^d, 陶金晶^a^,^b^,^c^,^d, 楚宇逸^a^,^b^,^c^,^d, 肖梅玲^a^,^b^,^c^,^d^,^e^,^*(), 刘长鹏^a^,^b^,^c^,^d^,^e^,^*(), 邢巍^a^,^b^,^c^,^d^,^e^,^*()

^a中国科学院长春应用化学研究所，先进电源实验室，吉林长春 130022，中国
^b中国科学技术大学应用化学与工程学院，安徽合肥 230026，中国
^c吉林省低碳化学电源重点实验室，吉林长春 130022，中国
^d中国科学院长春应用化学研究所，电分析化学国家重点实验室，吉林长春 130022，中国
^e中国科学院-香港氢能联合实验室，吉林长春 130022，中国

收稿日期:2025-06-18 修回日期:2025-07-09 接受日期:2025-07-31 发布日期:2025-07-31 出版日期:2025-09-28

Significantly Enhanced Oxygen Reduction Reaction Activity in Co-N-C Catalysts through Synergistic Boron Doping

Chang Lan^a^,^b^,^c^,^d, Jing-Sen Bai^a^,^b^,^c^,^d, Xin Guan^a^,^b^,^c^,^d, Shuo Wang^a^,^b^,^c^,^d, Nan-Shu Zhang^a^,^b^,^c^,^d, Yu-Qing Cheng^a^,^b^,^c^,^d, Jin-Jing Tao^a^,^b^,^c^,^d, Yu-Yi Chu^a^,^b^,^c^,^d, Mei-Ling Xiao^a^,^b^,^c^,^d^,^e^,^*(), Chang-Peng Liu^a^,^b^,^c^,^d^,^e^,^*(), Wei Xing^a^,^b^,^c^,^d^,^e^,^*()

^aLaboratory of Advanced Power Source, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, 130022, China
^bSchool of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei, 230026, China
^cJilin Province Key Laboratory of Low Carbon Chemical Power Sources, Changchun 130022, China
^dState Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese, Academy of Sciences, Changchun 130022, China
^eCIAC-HKUST Joint Laboratory for Hydrogen Energy, Changchun 130022, China

Received:2025-06-18 Revised:2025-07-09 Accepted:2025-07-31 Online:2025-07-31 Published:2025-09-28
Contact: * Meiling Xiao, E-mail: mlxiao@ciac.ac.cn (M.-L. Xiao), Changpeng Liu, E-mail: liuchp@ciac.ac.cn (C.-P. Liu), Wei Xing, E-mail: xingwei@ciac.ac.cn (W. Xing).

1. JOE2506181-Supporting Information.pdf(1824KB)

摘要/Abstract

摘要：

钴（Co）中心对含氧中间体的弱吸附能，是致使Co-N-C催化剂与昂贵的铂基催化剂在催化氧还原反应（ORR）中存在显著性能差异的主要原因。本研究通过硼酸铵共热解策略实现硼取代，从而对Co-N-C活性位点结构进行精准调控。反应中原位生成的氨气（NH₃）气体对表面进行刻蚀形成缺陷，为硼原子取代活性中心的氮原子奠定基础。精心构筑的CoB₁N₃活性中心可以赋予钴位点更高的电荷密度及与氧物种更强的吸附能，进而加速ORR动力学。如预期所示，所制备的Co-B/N-C催化剂展现出优于Co-N-C的ORR性能：半波电位提升40 mV，转换频率提高五倍。该催化剂优异的ORR活性在膜电极性能测试中同样显著，峰值功率密度达824 mW·cm^-2，取得了目前同等条件下钴基催化剂的最高水平。本工作不仅提供了先进催化剂的设计方法，更为燃料电池应用开发了一种极具前景的非贵金属ORR电催化剂。

关键词: 氧还原反应, 质子交换膜燃料电池, 单原子催化剂, Co-N-C, 硼掺杂

Abstract:

The weak adsorption energy of oxygen-containing intermediates on Co center leads to a considerable performance disparity between Co-N-C and costly Pt benchmark in catalyzing oxygen reduction reaction (ORR). In this work, we strategically engineer the active site structure of Co-N-C via B substitution, which is accomplished by the pyrolysis of ammonium borate. During this process, the in-situ generated NH₃ gas plays a critical role in creating surface defects and boron atoms substituting nitrogen atoms in the carbon structure. The well-designed CoB₁N₃ active site endows Co with higher charge density and stronger adsorption energy toward oxygen species, potentially accelerating ORR kinetics. As expected, the resulting Co-B/N-C catalyst exhibited superior ORR performance over Co-N-C counterpart, with 40 mV, and fivefold enhancement in half-wave potential and turnover frequency (TOF). More importantly, the excellent ORR performance could be translated into membrane electrode assembly (MEA) in a fuel cell test, delivering an impressive peak power density of 824 mW·cm^-2, which is currently the best among Co-based catalysts under the same conditions. This work not only demonstrates an effective method for designing advanced catalysts, but also affords a highly promising non-precious metal ORR electrocatalyst for fuel cell applications.

Key words: Oxygen reduction reaction, Proton exchange membrane fuel cell, Single-atom catalyst, Co-N-C, Boron doping

兰畅, 柏景森, 关欣, 王烁, 张楠淑, 程雨晴, 陶金晶, 楚宇逸, 肖梅玲, 刘长鹏, 邢巍. 协同硼掺杂显著提升Co-N-C催化剂的氧还原反应活性[J]. 电化学（中英文）, 2025, 31(9): 2506181.

Chang Lan, Jing-Sen Bai, Xin Guan, Shuo Wang, Nan-Shu Zhang, Yu-Qing Cheng, Jin-Jing Tao, Yu-Yi Chu, Mei-Ling Xiao, Chang-Peng Liu, Wei Xing. Significantly Enhanced Oxygen Reduction Reaction Activity in Co-N-C Catalysts through Synergistic Boron Doping[J]. Journal of Electrochemistry, 2025, 31(9): 2506181.

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链接本文: https://electrochem.xmu.edu.cn/CN/10.61558/2993-074X.3577

https://electrochem.xmu.edu.cn/CN/Y2025/V31/I9/2506181

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协同硼掺杂显著提升Co-N-C催化剂的氧还原反应活性

Significantly Enhanced Oxygen Reduction Reaction Activity in Co-N-C Catalysts through Synergistic Boron Doping

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