Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

过电位 催化作用 介孔材料 材料科学 沸石咪唑盐骨架 化学工程 析氧 纳米技术 电化学 碳纤维 金属有机骨架 咪唑酯 热解 电催化剂 可逆氢电极 电极 化学 无机化学 有机化学 工作电极 物理化学 吸附 复合材料 复合数 工程类
作者
Ruixue Zheng,Qinglei Meng,Hao Zhang,Teng Li,Di Yang,Li Zhang,Xiaolong Jia,Changpeng Liu,Jianbing Zhu,Xiaozheng Duan,Meiling Xiao,Wei Xing
出处
期刊:Journal of Energy Chemistry [Elsevier BV]
卷期号:90: 7-15 被引量:16
标识
DOI:10.1016/j.jechem.2023.10.045
摘要

Developing cost-effective, robust and stable non-precious metal catalysts for oxygen reduction reaction (ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries. Although Fe-N-C single atom catalysts (SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N4 sites, they suffer from serious mass transport limitations as microporous templates/substrates, i.e., zeolitic imidazolate frameworks (ZIFs), are usually employed to host the active sites. Motivated by this challenge, we herein develop a hydrogen-bonded organic framework (HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N4 sites. Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid (NH2-BDC) and p-phenylenediamine (PDA) as both soft templates and C, N precursors. Benefitting from the structural merits inherited from HOF templates, the optimized catalyst (denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V (vs. reversible hydrogen electrode (RHE)) and a small overpotential of 356 mV at 10 mA cm−2 for the oxygen evolution reaction (OER). More excitingly, its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge–discharge gap of 0.72 V after 160 h. Molecular dynamics (MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O2, thus enhancing the ORR performance. In situ Raman results further indicate that the conversion of O2 to *O2− the rate-determining step (RDS) for Fe-N-C SAC-950. This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.
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