Microporous 3D-Structured Hierarchically Entangled Graphene-Supported Pt3Co Alloy Catalyst for PEMFC Application with Process-Friendly Features,ACS Applied Materials & Interfaces

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Microporous 3D-Structured Hierarchically Entangled Graphene-Supported Pt3Co Alloy Catalyst for PEMFC Application with Process-Friendly Features
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-06-02 , DOI: 10.1021/acsami.3c03372
Narugopal Manna _{1,

2} , Mayank Singh _{1,

2} , Sreekumar Kurungot _{1,

2}

Affiliation

To improve the oxygen reduction reaction (ORR) performance in a proton-exchange membrane fuel cell (PEMFC) cathode with respect to mass activity and durability, a suitable electrocatalyst design strategy is essentially needed. Here, we have prepared a sub-three nm-sized platinum (Pt)–cobalt (Co) alloy (Pt₃Co)-supported N-doped microporous 3D graphene (Pt₃Co/pNEGF) by using the polyol synthesis method. A microwave-assisted synthesis method was employed to prepare the catalyst based on the 3D porous carbon support with a large pore volume and dense micro-/mesoporous surfaces. The ORR performance of Pt₃Co/pNEGF closely matches with the state-of-the-art commercial Pt/C catalyst in 0.1 M HClO₄, with a small overpotential of 10 mV. The 3D microporous structure of the N-doped graphene significantly improves the mass transport of the reactant and thus the overall ORR performance. As a result of the lower loading of Pt in Pt₃Co/pNEGF as compared to that in Pt/C, the alloy catalyst achieved 1.5 times higher mass activity than Pt/C. After 10,000 cycles, the difference in the electrochemically active surface area (ECSA) and half-wave potential (E_1/2) of Pt₃Co/pNEGF is found to be 5 m² g_Pt^–1 (ΔECSA) and 24 mV (ΔE_1/2), whereas, for Pt/C, these values are 9 m² g_Pt^–1 and 32 mV, respectively. Finally, in a realistic perspective, single-cell testing of a membrane electrode assembly (MEA) was made by sandwiching the Pt₃Co/pNEGF-coated gas diffusion layers as the cathode displayed a maximum power density of 800 mW cm^–2 under H₂–O₂ feed conditions with a clear indication of helping the system in the mass-transfer region (i.e., the high current dragging condition). The nature of the I–V polarization shows a progressively lower slope in this region of the polarization plot compared to a similar system made from its Pt/C counterpart and a significantly improved performance throughout the polarization region in the case of the system made from the Pt₃Co/NEGF catalyst (without the microwave treatment) counterpart. These results validate the better process friendliness of Pt₃Co/pNEGF as a PEMFC electrode-specific catalyst owing to its unique texture with 3D architecture and well-defined porosity with better structural endurance.

中文翻译：

用于 PEMFC 应用的微孔 3D 结构分层缠结石墨烯负载 Pt3Co 合金催化剂，具有工艺友好的特性

为了提高质子交换膜燃料电池 (PEMFC) 阴极在质量活性和耐久性方面的氧还原反应 (ORR) 性能，必须采用合适的电催化剂设计策略。在这里，我们通过使用多元醇合成方法制备了亚三纳米尺寸的铂 (Pt)-钴 (Co) 合金 (Pt ₃ Co) 负载的 N 掺杂微孔 3D 石墨烯 (Pt _{3 Co/pNEGF)。}采用微波辅助合成方法制备基于具有大孔体积和致密微/中孔表面的 3D 多孔碳载体的催化剂。_{Pt 3} Co/pNEGF在 0.1 M HClO ₄中的 ORR 性能与最先进的商用Pt/C 催化剂非常接近，具有 10 mV 的小过电势。N 掺杂石墨烯的 3D 微孔结构显着改善了反应物的传质，从而提高了整体 ORR 性能。由于与Pt/C 相比， Pt _{3 Co/pNEGF 中的 Pt 载量较低，合金催化剂的质量活性比 Pt/C 高 1.5 倍。}10,000 次循环后，发现Pt ₃ Co/pNEGF 的电化学活性表面积 (ECSA) 和半波电位 ( E _1/2 ) 的差异为 5 m ² g _Pt^–1 (ΔECSA) 和 24 mV ( Δ E _1/2 )，而对于 Pt/C，这些值为 9 m ² g _Pt^–1和 32 mV，分别。_{最后，从现实的角度来看，通过将 Pt 3} Co/pNEGF 涂层气体扩散层夹在中间对膜电极组件 (MEA) 进行单电池测试，因为阴极在 H 下显示出 800 mW cm ^{–2的最大功率密度}₂ –O ₂进料条件清楚地表明有助于系统进入传质区域（即高电流拖曳条件）。I - V极化的性质表明，与由其 Pt/C 对应物制成的类似系统相比，极化图的该区域的斜率逐渐降低，并且在由 Pt/C 制成的系统的情况下，整个极化区域的性能显着提高铂₃ Co/NEGF 催化剂（未经微波处理）对应物。_{这些结果证实了 Pt 3} Co/pNEGF 作为 PEMFC 电极专用催化剂具有更好的工艺友好性，因为其具有 3D 结构的独特纹理和明确定义的孔隙率以及更好的结构耐久性。

更新日期：2023-06-02

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