介孔碗状碳载体促进燃料电池阴极氧气传输

doi:10.1016/S1872-2067(24)60285-8

催化学报 ›› 2025, Vol. 72: 254-265.DOI: 10.1016/S1872-2067(24)60285-8

介孔碗状碳载体促进燃料电池阴极氧气传输

卢明佳^a^,^c^,¹, 梁锦辉^a^,¹, 曾彬文^a, 李威^a, 李蕴琪^b, 王庆鑫^b, 李钰怀^c, 陈泓^c, 李剑铮^c, 陈阳阳^a, 梁乐程^a, 杜丽^a, 相艳^b^,^*(), 廖世军^a^,^*(), 崔志明^a^,^*()

^a华南理工大学化学与化工学院, 广东省燃料电池技术重点实验室, 广东广州 510641
^b北京航空航天大学能源与动力工程学院, 仿生能源材料与器件北京市重点实验室, 多栖平台驱动系统全国重点实验室, 北京 100191
^c广州汽车集团股份有限公司汽车工程研究院, 广东省汽车清洁动力与能源应用技术重点实验室, 广东广州 511434

收稿日期:2024-10-14 接受日期:2025-02-23 出版日期:2025-05-18 发布日期:2025-05-20
通讯作者: *电子信箱: zmcui@scut.edu.cn (崔志明),chsjliao@scut.edu.cn (廖世军),xiangy@buaa.edu.cn (相艳).
作者简介:¹共同第一作者.
基金资助:
广东省重点技术研发计划(2023B0909060003);国家自然科学基金(22372062);国家自然科学基金(22072048);国家自然科学基金(U22A20419);广东省清洁汽车推进与能源应用技术重点实验室(2024B1212020006)

Mesoporous bowl-like carbon support for boosting oxygen transport of fuel cell cathode

Mingjia Lu^a^,^c^,¹, Jinhui Liang^a^,¹, Binwen Zeng^a, Wei Li^a, Yunqi Li^b, Qinqxin Wang^b, Yuhuai Li^c, Hong Chen^c, Jianzheng Li^c, Yangyang Chen^a, Lecheng Liang^a, Li Du^a, Yan Xiang^b^,^*(), Shijun Liao^a^,^*(), Zhiming Cui^a^,^*()

^aGuangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, Guangdong, China
^bNational Key Laboratory of Multi-perch Vehicle Driving Systems, Beijing Key Laboratory of Bio-inspired Energy Materials and Devices, School of Energy and Power Engineering, Beihang University, Beijing 100191, China
^cGAC automotive research & development center, Guangdong Provincial Key Laboratory of Clean Automotive Propulsion and Energy Application Technology, Guangzhou 511434, Guangdong, China

Received:2024-10-14 Accepted:2025-02-23 Online:2025-05-18 Published:2025-05-20
Contact: *E-mail: zmcui@scut.edu.cn (Z. Cui), chsjliao@scut.edu.cn (S. Liao), xiangy@buaa.edu.cn (Y. Xiang).
About author:¹ Contributed equally to this work.
Supported by:
key Technologies R&D Program of Guangdong Province(2023B0909060003);National Natural Science Foundation of China(22372062);National Natural Science Foundation of China(22072048);National Natural Science Foundation of China(U22A20419);Guangdong Provincial Key Laboratory of Clean Automotive Propulsion and Energy Application Technology(2024B1212020006)

摘要/Abstract

摘要：

质子交换膜燃料电池(PEMFC)具有高的能源转换效率以及零碳排放等优点, 被广泛认为是一种有前景的动力电源. 目前, 燃料电池阴极催化层普遍使用的是碳载铂基催化剂, 碳载体在实现催化剂均匀分散以及增强氧气传输等方面起到重要作用. 但由于阴极氧还原反应动力学较为缓慢, 因此需要高的铂载量(0.2-0.35 mg_pt cm^-2)以维持高的输出功率, 这成为燃料电池大规模应用的一个关键难题. 近年来, 为了降低阴极铂载量的同时维持性能, 大量的研究致力于开发各种先进的多孔碳载体, 但是由于孔径分布不集中导致质子和氧气在传质控制区(>1.5 A cm^-2)展现出较大的传质阻抗, 进而导致实际燃料电池展现出明显的电压衰减. 因此, 迫切需要开发具有特殊形貌以及合适孔结构(4-7 nm)的多孔碳载体以增强燃料电池的输出功率.

针对上述问题, 本文采用硬模板法制备了具有合适介孔结构的碗状碳, 即以正硅酸四乙酯为球形二氧化硅模板的前驱体, 然后通过表面聚合间苯二酚和甲醛的酚醛树脂(RF). 在间苯二酚和甲醛的聚合过程中, 小的二氧化硅颗粒被均匀地嵌入聚合物中, 形成核壳结构的SiO₂@SiO₂/RF. 酚醛树脂随后通过高温裂解转化为碳. 最后通过氢氟酸刻蚀去除二氧化硅模板, 碳壳在毛细力作用下通过球形壳的屈曲效应塌缩到内腔中, 从而形成多孔的碗状结构. 通过与空心碳球和实心碳球对比, 来探究碗状碳特殊形貌对氧气传输的作用. 采用X射线衍射、拉曼光谱、四探针电导率测试、氮气吸脱附曲线、扫描电镜和透射电镜等手段对其进行测试. 以碗状碳、空心碳球和实心碳球为载体合成了碳载的Pt₃Co金属间化合物催化剂, 并通过旋转圆盘电极及单电池考察了其电催化性能. 物理表征结果显示, 碗状碳载体具有高的比表面积(1200 m² g^-1)以及合适的孔径分布(~4 nm). 电化学测试表明, 相较于空心多孔碳球和固体实心碳球所负载的Pt₃Co催化剂以及商业Pt/C催化剂, 碗状碳负载的Pt₃Co催化剂(Pt₃Co/BC)的性能显著提升. 在所研究的催化剂中, Pt₃Co/BC催化剂的MEA表现出最佳的H₂-空气燃料电池性能, 阴极催化层载量为0.2 mg_pt cm^-2, 在0.6 V时, 产生1.3 A cm^-2的最大电流密度; 在1.5 A cm^-2时, 它能产生0.5 V的最高工作电位. 实验结果以及仿真模拟表明, Pt₃Co/BC催化剂的高活性来自于碗状碳具有特殊的形貌以及合适的孔结构可以促进催化剂的均匀分散以及增强氧气传输.

开发具有特殊形貌以及合适孔结构的碳载体对提升燃料电池的输出功率至关重要, 其中具有孔径约为4 nm的介孔碳载体有望实现具有低铂载量的高性能燃料电池. 该研究揭示了碳载体形貌以及孔结构对氧气传输的影响, 为新型多孔碳载体的开发提供新思路.

关键词: 燃料电池, 氧还原, 传质, 载体, 碗状碳

Abstract:

The development of advanced support is conducive to promoting the practical application of fuel cells but remains an enormous challenge in terms of stabilizing catalyst particles and enabling improved accessibility to O₂. Beyond solid carbon black and conventional porous carbon, we demonstrate a new type of mesoporous bowl-like carbon support with a high specific surface area of over 1200 m² g^-1 and ~ 4 nm pore. Both rotating disk electrode and membrane electrode assembly (MEA) tests show that BC-supported Pt₃Co (Pt₃Co/BC) catalyst greatly outperforms hollow porous carbon spheres and solid carbon spheres supported Pt₃Co catalysts. The Pt₃Co/BC catalysts exhibited remarkable performance as cathode catalyst in MEA, achieving a comparable open-circuit voltage of approximately 0.95 V under H₂-air condition and a current density of 1.3 A cm^-2 at 0.6 V with a loading of only 0.2 mg_Pt cm^-2. Diffusion simulations and physical characterizations demonstrate that the high porosity and highly accessible pore structure of BC support facilitate the uniform distribution of catalyst particles and enhance the mass transport of O₂, thereby resulting in a significant improvement in catalytic activity and durability. This work provides new insights into the influence of support shape on mass transport of reactants and electrochemical performances of the catalyst in MEA.

Key words: Fuel cell, Oxygen reduction reaction, Mass transport, Support, Bowl-like carbon

卢明佳, 梁锦辉, 曾彬文, 李威, 李蕴琪, 王庆鑫, 李钰怀, 陈泓, 李剑铮, 陈阳阳, 梁乐程, 杜丽, 相艳, 廖世军, 崔志明. 介孔碗状碳载体促进燃料电池阴极氧气传输[J]. 催化学报, 2025, 72: 254-265.

Mingjia Lu, Jinhui Liang, Binwen Zeng, Wei Li, Yunqi Li, Qinqxin Wang, Yuhuai Li, Hong Chen, Jianzheng Li, Yangyang Chen, Lecheng Liang, Li Du, Yan Xiang, Shijun Liao, Zhiming Cui. Mesoporous bowl-like carbon support for boosting oxygen transport of fuel cell cathode[J]. Chinese Journal of Catalysis, 2025, 72: 254-265.

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图/表 6

Scheme 1. Schematic illustrating the synthesis of BC, HPCS and CS support.

Fig. 1. SEM image (a-c), nitrogen adsorption-desorption isotherms (d), and conductivity diagram (e) of BC, HPCS, and CS. (f) XRD patterns of Pt3Co/BC, Pt3Co/HPCS, Pt3Co/CS, and Pt/C.

Fig. 2. (a,b) TEM image of Pt3Co/BC. (c,d) TEM image of Pt3Co/HPCS. (e,f) TEM images of Pt3Co/CS, and particle size distribution map in the inset. (g) Atomic resolution HAADF-STEM image of Pt3Co NP. (h) Crop of the superlattice feature in (g). (i) Line scans of a single Pt3Co nanoparticle. Blue-colored atom is Pt, yellow colored is Co.

Fig. 3. (a) CVs of different electrocatalysts in 0.1 mol L?1 HClO4 solution. (b) ORR polarization curves in O2-saturated 0.1 mol L?1 HClO4. Rotation rate:1600 r min?1; sweep rate:10 mV s?1. (c) Histogram of mass and specific activities of different electrocatalysts. (d?f) ORR polarization curves before and after ADT for Pt3Co/BC, Pt3Co/HPCS, and Pt3Co/CS, the inset shows enlarged views of the area near 0.8?0.94 V. TEM images and the histograms of particle size distribution maps for Pt3Co/BC (g), Pt3Co/HPCS (h), and Pt3Co (i) after ADT.

Fig. 4. Electrochemical performance test on MEA. (a) H2-air fuel polarization plots and power density plots. (b) Nyquist plots of Pt3Co/BC measured at 800 mA cm-2 under 100%RH. (c) Catalytic layer porosity of Pt3Co/BC, Pt3Co/HPCS, Pt3Co/CS and Pt/C. The SEM of MEA with the Pt3Co/BC (d), Pt3Co/HPCS (e), and Pt3Co/CS (f) catalyst as cathodes.

Fig. 5. (a) COMSOL Multiphysics Modeling of O2 diffusion into cathode catalytic layer consisting of three catalysts, respectively. Enlarged O2 diffusion images of Pt3Co/BC (b), Pt3Co/HPCS (c), and Pt3Co/CS (d). (e) Distribution of O2 diffusion concentration for Pt3Co/BC, Pt3Co/HPCS, and Pt3Co/CS at identical point.

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介孔碗状碳载体促进燃料电池阴极氧气传输

Mesoporous bowl-like carbon support for boosting oxygen transport of fuel cell cathode

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[1]	纳国豪, 郑红顺, 陈明鹏, 孙华传, 吴阅文, 李德全, 陈赟, 赵勃然, 赵博, 周桐, 何天威, 张雨潇, 赵建红, 张裕敏, 张瑾, 刘锋, 崔浩, 柳清菊. Pt原位还原诱导NiFe-MOF拓扑转变用于工业级电解海水制氢[J]. 催化学报, 2025, 72(5): 211-221.
[2]	李思明, 孙恩样, 魏鹏飞, 赵微, 裴随珠, 陈颖, 杨洁, 陈绘丽, 尹熙, 王旻, 李亚伟. 浸渍离子液体于多孔Fe-N-C电催化剂以改善聚合物电解质燃料电池电极动力学与质量传输[J]. 催化学报, 2025, 72(5): 277-288.
[3]	马军, 徐冰, 曹硕, 李世艳, 储伟, Siglinda Perathoner, Gabriele Centi, 刘岳峰. 反应条件下Ni/Mo₂CT_x MXene催化剂结构演变调节CO₂还原性能[J]. 催化学报, 2025, 72(5): 243-253.
[4]	吴君, 刘立乾, 严鑫悦, 潘刚, 白家豪, 王成兵, 李福伟, 李永. 用于生物质基香草醛水相高选择性加氢脱氧的氮掺杂中空碳球负载Pd催化剂的微环境设计和构筑[J]. 催化学报, 2025, 71(4): 267-284.
[5]	陈繁荣, 傅佳驹, 丁亮, 卢晓英, 蒋哲, 张小玲, 胡劲松. 硫锚定策略提升亚3纳米In₂S₃纳米颗粒电还原CO₂至甲酸盐的稳定性[J]. 催化学报, 2025, 71(4): 138-145.
[6]	段会梅, 李晓菲, 王传辉, 张丛筠, 余楷文, 陈磊, 张云尚, 纪嘉宾, 杨贤峰, 杨东江. Ir/TiO₂催化剂甲烷燃烧反应中TiO₂晶面依赖效应[J]. 催化学报, 2025, 70(3): 378-387.
[7]	李家欣, 吕燕, 吴雪岩, 郭新玉, 杨卓君, 郭继玺, 周天华, 贾殿赠. 分级结构NiO纳米管/纳米片表面限域生长Pt亚纳米团簇催化剂用于尿素辅助节能产氢[J]. 催化学报, 2025, 69(2): 203-218.
[8]	李阳阳, 杨静怡, 乔波涛, 张涛. 尺寸依赖的金属载体相互作用调控Pt/CoFe₂O₄催化反应性能[J]. 催化学报, 2025, 69(2): 292-302.
[9]	夏兵全, 刘高雄, 樊坤, 陈润东, 刘欣, 李来全. 基于双氧还原中心的共价三嗪框架构建的1D/2D S型异质结促进过氧化氢光合作用[J]. 催化学报, 2025, 69(2): 315-326.
[10]	贡立圆, 陶李, 王雷, 符显珠, 王双印. 高温质子交换膜燃料电池阴极抗磷酸中毒催化剂的研究进展[J]. 催化学报, 2025, 68(1): 155-176.
[11]	沈辰阳, 刘梦辉, 何松, 赵海波, 刘昌俊. 二氧化碳甲烷化负载型钌基催化剂的研究进展[J]. 催化学报, 2024, 63(8): 1-15.
[12]	梁腾, 李雨彤, 徐帅, 姚宇欣, 许荣萍, 边辑, 张紫晴, 井立强. 电荷迁移方向调控的BiVO₄量子点/苝四羧酸Z型异质结与纳米金修饰在人工光合成H₂O₂中的协同作用[J]. 催化学报, 2024, 62(7): 277-286.
[13]	陈瑞, 方翔, 张东方, 赫兰齐, 吴胤龙, 孙成华, 王昆, 宋树芹. 原位构筑三维有序自支撑Co-N-C一体化电极并用于高效电催化氧还原反应[J]. 催化学报, 2024, 61(6): 237-246.
[14]	孟爱云, 马辛源, 温达, 钟威, 周双, 苏耀荣. 高选择性H₂O₂光合成: Ba原子注入面内高度有序结晶结构的g-C₃N₄纳米棒[J]. 催化学报, 2024, 60(5): 231-241.
[15]	杨志远, 张燕, 肖娟定, 王俊英, 王俊中. 铋牺牲法制备石墨烯负载Fe-N单原子位点增效氧还原催化和锌-空气电池性能[J]. 催化学报, 2024, 59(4): 272-281.