空心共价有机框架衍生碳载体提升PtCo合金催化剂在燃料电池氧还原反应中的活性与稳定性

doi:10.1016/S1872-2067(26)64973-X

催化学报 ›› 2026, Vol. 83: 294-307.DOI: 10.1016/S1872-2067(26)64973-X

空心共价有机框架衍生碳载体提升PtCo合金催化剂在燃料电池氧还原反应中的活性与稳定性

李宫^a^,^b, 柏景森^a^,^b, 王丹^d, 梁亮^b^,^c, 汝春宇^d, 宫雪^d, 邵敏华^e^,^f^,^g^,^*(), 刘长鹏^a^,^b^,^c^,^*(), 肖梅玲^a^,^b^,^c^,^*(), 邢巍^a^,^b^,^c^,^*()

^a中国科学技术大学应用化学与工程学院, 安徽合肥 230026
^b中国科学院长春应用化学研究所, 低碳化学电力吉林省重点实验室, 吉林省氢能科技创新中心, 吉林长春 130022
^c中科院-香港科技大学氢能联合实验室, 吉林长春 130022
^d中国一汽集团研发总院发动机开发部, 吉林长春 130013
^e香港科技大学化学与生物工程系, 香港九龙 999077
^f香港科技大学能源研究院, 中科院-港科大氢能联合实验室, 香港九龙 999077
^g香港科技大学霍英东研究院, 广东广州 511458

收稿日期:2025-08-19 接受日期:2025-10-18 出版日期:2026-04-18 发布日期:2026-03-04
通讯作者: * 电子信箱: kemshao@ust.hk (邵敏华), liuchp@ciac.ac.cn (刘长鹏), mlxiao@ciac.ac.cn (肖梅玲), xingwei@ciac.ac.cn (邢巍).
基金资助:
国家自然科学基金(22272160);国家自然科学基金(U23A20137);长春市科技发展计划(23GZZ02);吉林省科技发展计划(20220301011GX);吉林省重大科技项目(222648GX0105103875);香港研究资助局(C6011-20GF);香港研究资助局(JLFS/P-602/24)

Hollow COF-derived carbon supports enable PtCo alloy catalysts with exceptional activity and durability for oxygen reduction reaction in fuel cells

Gong Li^a^,^b, Jingsen Bai^a^,^b, Dan Wang^d, Liang Liang^b^,^c, Chunyu Ru^d, Xue Gong^d, Minhua Shao^e^,^f^,^g^,^*(), Changpeng Liu^a^,^b^,^c^,^*(), Meiling Xiao^a^,^b^,^c^,^*(), Wei Xing^a^,^b^,^c^,^*()

^aSchool of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, Anhui, China
^bState Key Laboratory of Electroanalytic Chemistry, Jilin Province Key Laboratory of Low Carbon Chemistry Power, Jilin Provincial Science and Technology Innovation Center of Hydrogen Energy, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, Jilin, China
^cCIAC-HKUST Joint Laboratory for Hydrogen Energy, Changchun 130022, Jilin, China
^dEngine Development Department, General Institute of FAW, Changchun 130013, Jilin, China
^eDepartment of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Hong Kong 999077, China
^fCIAC-HKUST Joint Laboratory for Hydrogen Energy, Energy Institute, The Hong Kong University of Science and Technology, Hong Kong 999077, China
^gGuangzhou Key Laboratory of Electrochemical Energy Storage Technologies, Fok Ying Tung Research Institute, The Hong Kong University of Science and Technology, Guangzhou 511458, Guangdong, China

Received:2025-08-19 Accepted:2025-10-18 Online:2026-04-18 Published:2026-03-04
Contact: * E-mail: kemshao@ust.hk (Minhua Shao), liuchp@ciac.ac.cn (C. Liu), mlxiao@ciac.ac.cn (M. Xiao), xingwei@ciac.ac.cn (W. Xing).
Supported by:
National Natural Science Foundation of China(22272160);National Natural Science Foundation of China(U23A20137);Changchun Science and Technology Development Program(23GZZ02);Jilin Province Science and Technology Development Program(20220301011GX);Jilin Province Science and Technology Major Project(222648GX0105103875);Hong Kong Research Grant Council(C6011-20GF);Hong Kong Research Grant Council(JLFS/P-602/24)

摘要/Abstract

摘要：

质子交换膜燃料电池(PEMFC)因其高能量转化效率和零污染排放特性, 在交通运输及分布式能源领域具有重要应用前景. 然而, 阴极氧还原反应(ORR)动力学缓慢且催化剂稳定性不足, 仍是制约PEMFC商业化应用的关键瓶颈. Pt基合金催化剂虽表现出优异的本征活性, 但在酸性环境下, 催化剂通常面临Co溶出、颗粒团聚和载体腐蚀等失活问题. 近年来, 共价有机框架(COF)以其高度有序的结构、可调的功能位点和优异的多功能性, 成为制备高性能碳载体的理想前驱体. 基于COF衍生碳材料构建空心的限域结构, 可有效提升Pt利用率与耐久性, 但其普适性可控合成及结构调控仍具挑战性. 针对上述问题, 本工作提出一种简单、普适的空心COF(HCOF)衍生碳载体构筑策略, 为高活性高稳定燃料电池催化剂的开发提供新思路.
本文采用溶剂蒸发法快速制备了具有高结晶度的席夫碱型COF前驱体(如TAPTA-BTCA-COF), 通过Fenton反应生成的羟基自由基, 实现了C=N键的可控氧化断裂, 从而构筑出结构完整、壳层可调的空心COF(HCOF). 经高温碳化后, 得到具有空心限域结构的N掺杂碳载体, 并负载PtCo合金纳米颗粒, 形成PtCo@NC_TAPBT等系列催化剂. 透射电镜与X射线衍射分析表明, 所得催化剂保持完整的空心结构, 合金纳米颗粒(约3 nm)均匀分布于碳壳内, 表现出良好的空间限域与金属-载体相互作用. X-射线光电子能谱与扩展X-射线吸收精细结构分析显示, 空心壳层中的吡啶氮与石墨氮可与Pt发生电子耦合, 调节其d带中心, 从而优化氧中间体的吸附能. 旋转圆盘电极测试表明, PtCo@NC_TAPBT的半波电位达0.925 V (比商用Pt/C正移45 mV), 质量活性为1.46 A mg_Pt^-1, 是商用Pt/C的约10倍. 加速耐久性测试后, 其E_1/2几乎无衰减, 质量活性保持率高达87.7%, Pt与Co溶出率分别仅为9.8%与20.2%, 显示出显著的抗溶解与抗团聚能力. 在膜电极组件测试中, PtCo@NC_TAPBT在H₂-Air条件下峰值功率密度达1.23 W cm^-2, 质量活性(1.06 A mg_Pt^-1)超过美国能源部2025年目标的2.4倍; 电压衰减仅8 mV (30000次循环), 远优于Pt/C (30 mV). 此外, 空心碳壳的多级孔道结构显著降低氧传输阻力(R_tot = 69.9 S m^-1), 提高反应物扩散与水排出效率. 机制上, 空心结构通过空间限域抑制合金团聚, 同时N掺杂碳载体调控电子结构, 协同增强ORR活性与耐久性.
综上, 本研究提出的空心COF衍生碳载体构筑策略, 不仅在PtCo合金催化体系中实现了兼具高活性与高稳定性的电催化性能, 更为COF材料在燃料电池电极催化中的工程化应用提供了新方向. 该工作为开发低贵金属、高性能ORR催化剂提供了可推广的设计范式与理论依据.

关键词: 共价有机框架, 合金, 空心结构, 氧还原反应, 燃料电池

Abstract:

The development of high-performance and durable oxygen reduction reaction catalysts under harsh working environments remains a key challenge in advancing proton exchange membrane fuel cells. Here, we report a series of hollow-structured covalent organic framework-derived carbon as support materials for PtCo alloy nanocatalysts. These hollow architectures provide unique spatial confinement and encapsulation effects, which not only facilitate efficient mass transport but also protect active sites from degradation in acidic media, thereby ensuring simultaneous enhancement in activity and stability. The optimized PtCo@NC_TAPBT catalyst delivers a peak power density of 1.23 W cm^-2 under H₂-Air conditions and a mass activity of 1.06 A mg_Pt^-1 at 0.9 V, representing 2.41 times higher than that of commercial Pt/C (0.40 A mg_Pt^-1). Moreover, the fuel cell assembled with this catalyst exhibits outstanding durability, showing a voltage degradation of only 8 mV after 30000 cycles at 0.8 A cm^-2 and a mass activity retention of 87.7% (0.93 A mg_Pt^-1). Notably, this performance exceeds the U.S. Department of Energy’s 2025 initial mass activity target (0.44 A mg_Pt^-1) by a factor of 2.1, highlighting the potential of HCOF-derived carbon materials for next-generation fuel cell applications.

Key words: Covalent organic framework, Alloy, Encapsulation structure, Oxygen reduction reaction, Fuel cell

李宫, 柏景森, 王丹, 梁亮, 汝春宇, 宫雪, 邵敏华, 刘长鹏, 肖梅玲, 邢巍. 空心共价有机框架衍生碳载体提升PtCo合金催化剂在燃料电池氧还原反应中的活性与稳定性[J]. 催化学报, 2026, 83: 294-307.

Gong Li, Jingsen Bai, Dan Wang, Liang Liang, Chunyu Ru, Xue Gong, Minhua Shao, Changpeng Liu, Meiling Xiao, Wei Xing. Hollow COF-derived carbon supports enable PtCo alloy catalysts with exceptional activity and durability for oxygen reduction reaction in fuel cells[J]. Chinese Journal of Catalysis, 2026, 83: 294-307.

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Fig. 1. (a) Schematic illustration of the synthesis procedure of TAPB-BTCA-HCOF. (b) TEM images of TAPTA-BTCA-COF. (c) TEM images of TAPB-BTCA-HCOF. (d) XRD patterns of TAPTA-BTCA-COF and TAPTA-BTCA-HCOF. (e) FT-IR spectra of TAPTA-BTCA-COF and TAPTA-BTCA-HCOF.

Fig. 2. TEM images of PtCo@NCTPDV (a), PtCo@NCTPTF (b) and PtCo@NCTAPBT (c). STEM images of PtCo@NCTPDV (d), PtCo@NCTPTF (e) and PtCo@NCTAPBT (f) (the enclosure of ultrafine nanoparticle by HCOF indicated by white arrows). (g) XRD patterns of PtCo@NCTPDV, PtCo@NCTPTF and PtCo@NCTAPBT. (h) XRD patterns of PtCo@NCTAPBT annealing at different temperatures. (i) N2 adsorption-desorption isotherms of PtCo@NCTAPBT.

Fig. 3. (a) High-resolution XPS spectra Pt 4f of PtCo@NCTPDV, PtCo@NCTPTF and PtCo@NCTAPBT. (b) High-resolution XPS spectra N 1s of PtCo@NCTPDV, PtCo@NCTPTF and PtCo@NCTAPBT. Pt L3-edge (c) and Co K-edge (d) XANES spectra of PtCo@NCTPDV, PtCo@NCTPTF and PtCo@NCTAPBT with metal foils as references. Insert: image from the partially enlarged view. Fourier transforms of k3-weight Pt L3-edge (e) and Co K-edge (f) EXAFS spectra for PtCo@NCTPDV, PtCo@NCTPTF and PtCo@NCTAPBT, Pt foil and Co foil. (g) Wavelet transforms for the Pt L3-edge EXAFS data of PtCo@NCTPDV, PtCo@NCTPTF, PtCo@NCTAPBT and Pt foil.

Fig. 4. (a) ORR polarization curves of PtCo@NCTPDV, PtCo@NCTPTF, PtCo@NCTAPBT and Pt/C. (b) The corresponding Tafel plots of PtCo@NCTPDV, PtCo@NCTPTF, PtCo@NCTAPBT and Pt/C. (c) Comparison of MA and SA for PtCo@NCTAPBT and Pt/C at 0.90 V (vs. RHE). (d) ORR polarization curves of PtCo@NCTAPBT and Pt/C before and after 50k. (e) Cyclic voltammetry curve of PtCo@NCTAPBT before and after ADT 50k. (f) The electron transfer number (n) at different potentials (left) and HO2? yield (right) for PtCo@NCTAPBT and Pt/C catalysts.

Fig. 5. Polarization and power density curves of PtCo@NCTPDV, PtCo@NCTPTF, PtCo@NCTAPBT and Pt/C in H2-O2 fuel cells (a) and H2-Air fuel cells (b) at 80 °C with 200 kPa back pressure and 100% Relative Humidity (RH) with the cathode metal loading of 0.1 mgPt cm?2. (c) Rtot of the cathode for PtCo@NCTAPBT PtCo@NCTAPBT-COF and Pt/C in the PEMFC at various total cathode pressures. (d) Polarization and power density curves of PtCo@NCTAPBT in H2-O2 fuel cells at 80 °C with the back pressure of 200 kPa and 100% RH with the cathode metal loading of 0.1 mgPt cm?2 after 30k potential cycles. (e) MA at 0.9 V and voltage loss at 0.8 A cm?2 at the begin of life (BOL), 10k and 30k. Note: the purple and yellow dashed lines indicate DOE targets for MA at BOL and end of life (EOL) after 30k potential cycles, respectively. The blue dashed line indicates the DOE target for voltage drop at 0.8 A cm?2 after 30k potential cycles. (f) Comparison of stability retain and MA after load cycles between PtCo@NCTAPBT with the state-of-art in the literature. (f) Current density as a function of time for PtCo@NCTAPBT with a 0.1 mgPt?cm?2 loading at 0.6 V in H2-Air conditions.

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空心共价有机框架衍生碳载体提升PtCo合金催化剂在燃料电池氧还原反应中的活性与稳定性

Hollow COF-derived carbon supports enable PtCo alloy catalysts with exceptional activity and durability for oxygen reduction reaction in fuel cells

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