Rational design and synthesis of three-dimensional hierarchical porous Fe–N co-doped graphene as a high performance electrocatalyst for oxygen reduction reaction

IF 3.2 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR

Journal of Solid State Chemistry Pub Date : 2025-07-19 DOI:10.1016/j.jssc.2025.125530

Tingwei Zhang , Haixu Wang , Bo Peng , Tiechun Li , Zhongfang Li

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Abstract

Exploring non-precious metal electrocatalysts that are low-cost, highly active, and durable is essential for the large-scale commercialization of fuel cells. In this study, a cost-effective approach for preparing Fe–N co-doped three-dimensional (3D) graphene catalysts with a hierarchical microporous-mesoporous-macroporous structure has been reported. It was achieved using Poly (2,2'-(m-phenyl)-5,5′-bibenzimidazole) (MPBI) as both the nitrogen and carbon source, and CaCO₃ as a template. Due to the synergistic interaction between the extensively distributed Fe-N_X active sites and the 3D hierarchical porous graphene framework, the resulting Fe–N/3DG#2 catalyst demonstrated superior oxygen reduction reaction (ORR) performance. The half-wave potential of Fe–N/3DG#2 (0.863 V vs. RHE) exceeded that of 20 wt% Pt/C (0.851 V vs. RHE). Moreover, accelerated durability tests and i-t chronoamperometry measurements revealed that Fe–N/3DG#2 exhibited significantly improved durability compared to 20 wt% Pt/C.

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合理设计合成三维分层多孔Fe-N共掺杂石墨烯作为氧还原反应的高性能电催化剂

探索低成本、高活性和耐用的非贵金属电催化剂对于燃料电池的大规模商业化至关重要。在这项研究中，报道了一种经济有效的方法来制备具有微孔-介孔-大孔结构的Fe-N共掺杂三维（3D）石墨烯催化剂。以聚（2,2'-（m-苯基）-5,5 '-双苯并咪唑）（MPBI）为氮源和碳源，CaCO3为模板剂实现了该反应。由于广泛分布的Fe-NX活性位点与三维分层多孔石墨烯框架之间的协同作用，得到的Fe-N /3DG#2催化剂表现出优异的氧还原反应（ORR）性能。Fe-N /3DG#2的半波电位（0.863 V vs. RHE）超过了20% wt% Pt/C的半波电位（0.851 V vs. RHE）。此外，加速耐久性测试和i-t计时电流测量显示，与20% Pt/C相比，Fe-N /3DG#2的耐久性显着提高。

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来源期刊

Journal of Solid State Chemistry 化学-无机化学与核化学

CiteScore

6.00

自引率

9.10%

发文量

848

审稿时长

25 days

期刊介绍： Covering major developments in the field of solid state chemistry and related areas such as ceramics and amorphous materials, the Journal of Solid State Chemistry features studies of chemical, structural, thermodynamic, electronic, magnetic, and optical properties and processes in solids.