Wettability，Adhesion and Mass Transfer of the Active Site within Fe-N-C Catalyst for Proton Exchange Membrane Fuel Cells

HUANG Dong; GENG Limin; LÜ Qiang

doi:10.7652/xjtuxb202510014

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Wettability，Adhesion and Mass Transfer of the Active Site within Fe-N-C Catalyst for Proton Exchange Membrane Fuel Cells

更新时间：2025-09-28

- Wettability，Adhesion and Mass Transfer of the Active Site within Fe-N-C Catalyst for Proton Exchange Membrane Fuel Cells
- Journal of Xi'an Jiaotong University Vol. 59, Issue 10, Pages: 148-159(2025)
- 作者机构：
- 作者简介：
- 基金信息：
- DOI：10.7652/xjtuxb202510014
  CLC： TK91
- Received：28 February 2025，
  
  Published：10 October 2025
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HUANG Dong, GENG Limin, LÜ Qiang. Wettability，Adhesion and Mass Transfer of the Active Site within Fe-N-C Catalyst for Proton Exchange Membrane Fuel Cells[J]. Journal of Xi'an Jiaotong University, 2025, 59(10): 148-159.
DOI：

HUANG Dong, GENG Limin, LÜ Qiang. Wettability，Adhesion and Mass Transfer of the Active Site within Fe-N-C Catalyst for Proton Exchange Membrane Fuel Cells[J]. Journal of Xi'an Jiaotong University, 2025, 59(10): 148-159. DOI： 10.7652/xjtuxb202510014.

摘要

为考察质子交换膜燃料电池非贵金属催化剂Fe-N-C构成的阴极催化层三相界面稳定性和传质性能，以沸石咪唑酯骨架结构材料（ZIF-8）为前驱体，引入氧化

石墨烯，在800～1200℃温度范围内采用热合成方法制备了一系列Fe-N-C催化剂，通过电化学测试和形貌表征，筛选出氧还原反应催化活性最佳的组别，并分析了其代表性活性位点Fe

N。通过分子动力学模拟，探究了包含Fe

N的阴极催化层三相界面内部传质过程以及决定该结构稳定性的活性位点表面润湿能力及其与离聚物间黏附性。研究结果表明：1000℃热解获得的Fe-N-C-1000催化剂具有最佳催化活性，其极限电流密度为5.18mA/cm

，半波电位为0.86mV，反应以4电子途径进行；Fe-N-C-1000继承了ZIF-8的十二面体结构，且存在大量孔径约3.9nm的介孔，其代表性活性位点为Fe

N；在298、358K下，Fe

N活性位点表面呈现良好亲水性，无论平整表面或纳米颗粒结构，Fe

N和Nafion离聚物间的黏附性均强于Pt；在包含Fe

N的三相界面中，H

和O

的扩散系数显著高于Pt/C催化剂三相界面；Fe

N纳米颗粒对H

和O

也具有更强吸附能力。该研究结果可为Fe-N-C催化剂活性位点筛选和分子尺度性能评估提供参考。

Abstract

To investigate the stability andmass transfer performance of the three-phase interface in the cathode catalytic layer of proton exchangemembrane fuel cells (PEMFCs) using nonpreciousmetal Fe-N-C catalysts

a series of Fe-N-C catalysts are synthesized via pyrolysis at temperatures ranging from 800—1200 ℃

using zeolitic imidazolate framework (ZIF-8) as a precursor with the introduction of graphene oxide. The optimal catalyst for oxygen reduction reaction activity is selected through electrochemical testing andmorphological characterization

and its representative active site

is analyzed. Molecular dynamics simulations are employed to explore themass transfer processes within the three-phase interface of the cathode catalytic layer containing Fe

as well as the wettability of the active site surface

which determine the structural stability

and its adhesion to the ionomer. The results show that the Fe-N-C-1000 catalyst obtained at 1000℃ exhibits the best catalytic activity

with a limiting current density of 5.18mA/cm

a half-wave potential of 0.86V

and a 4-electron reaction pathway. Fe-N-C-1000 inherits the dodecahedral structure of ZIF-8 and contains a large number ofmesopores with an average pore size of approximately 3.9nm

with Fe

N as the represe

ntative active site. At 298K and 358K

the Fe

N active site surface demonstrates excellent hydrophilicity

and its adhesion to Nafion ionomer is stronger than that of Pt

regardless of whether the surface is flat or nanoparticlestructured. Within the three-phase interface containing Fe

the diffusion coefficients of H

and O

are significantly higher than those in the Pt/C three-phase interface. Additionally

N nanoparticles exhibit stronger adsorption capabilities for H

and O

.This study provides valuable insights for the screening andmolecular-scale performance evaluation of Fe-N-C catalyst active sites.

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