Department of Sciences & Humanities, Rajiv Gandhi Institute of Petroleum Technology (RGIPT), Jais, Amethi, Uttar Pradesh 229304, India.
Department of Physics, National Institute of Technology, Durgapur 713209, West Bengal, India.
Inorg Chem. 2023 May 29;62(21):8200-8209. doi: 10.1021/acs.inorgchem.3c00584. Epub 2023 May 17.
Developing nonprecious metal-based oxygen reduction reaction (ORR) electrocatalysts with superior activity and durability is crucial for commercializing proton-exchange membrane (PEM) fuel cells. Herein, we report a metal-organic framework (MOF)-derived unique N-doped hollow carbon structure (NiCo/hNC), comprising of atomically dispersed single-Ni-atom (NiN) and small NiCo alloy nanoparticles (NPs), for highly efficient and durable ORR catalysis in both alkaline and acidic electrolytes. Density functional theory (DFT) calculations reveal the strong coupling between NiN and NiCo NPs, favoring the direct 4e transfer ORR process by lengthening the adsorbed O-O bond. Moreover, NiCo/hNC as a cathode electrode in PEM fuel cells delivered a stable performance. Our findings not only furnish the fundamental understanding of the structure-activity relationship but also shed light on designing advanced ORR catalysts.
开发具有优异活性和耐久性的非贵金属氧还原反应（ORR）电催化剂对于质子交换膜（PEM）燃料电池的商业化至关重要。在此，我们报告了一种金属有机骨架（MOF）衍生的独特氮掺杂中空碳结构（NiCo/hNC），其包含原子分散的单镍原子（NiN）和小的 NiCo 合金纳米颗粒（NPs），可在碱性和酸性电解质中实现高效且耐用的 ORR 催化。密度泛函理论（DFT）计算揭示了 NiN 和 NiCo NPs 之间的强耦合，通过延长吸附的 O-O 键，有利于直接的 4e 转移 ORR 过程。此外，NiCo/hNC 作为 PEM 燃料电池中的阴极电极表现出稳定的性能。我们的研究结果不仅提供了对结构-活性关系的基本理解，也为设计先进的 ORR 催化剂提供了思路。
