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从金属有机框架到单原子铁植入的氮掺杂多孔碳:在碱性和酸性介质中均实现高效氧还原

From Metal-Organic Frameworks to Single-Atom Fe Implanted N-doped Porous Carbons: Efficient Oxygen Reduction in Both Alkaline and Acidic Media.

作者信息

Jiao Long, Wan Gang, Zhang Rui, Zhou Hua, Yu Shu-Hong, Jiang Hai-Long

机构信息

Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Soft Matter Chemistry, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.

Materials Science Division, Advanced Photon Source, Argonne National Laboratory, Lemont, IL, 60439, USA.

出版信息

Angew Chem Int Ed Engl. 2018 Jul 9;57(28):8525-8529. doi: 10.1002/anie.201803262. Epub 2018 Jun 12.

Abstract

It remains highly desired but a great challenge to achieve atomically dispersed metals in high loadings for efficient catalysis. Now porphyrinic metal-organic frameworks (MOFs) have been synthesized based on a novel mixed-ligand strategy to afford high-content (1.76 wt %) single-atom (SA) iron-implanted N-doped porous carbon (Fe -N-C) via pyrolysis. Thanks to the single-atom Fe sites, hierarchical pores, oriented mesochannels and high conductivity, the optimized Fe -N-C exhibits excellent oxygen reduction activity and stability, surpassing almost all non-noble-metal catalysts and state-of-the-art Pt/C, in both alkaline and more challenging acidic media. More far-reaching, this MOF-based mixed-ligand strategy opens a novel avenue to the precise fabrication of efficient single-atom catalysts.

摘要

在高负载量下实现原子分散的金属以进行高效催化,这仍然是人们非常渴望的,但也是一个巨大的挑战。目前,基于一种新型混合配体策略合成了卟啉金属有机框架(MOF),通过热解得到高含量(1.76 wt %)的单原子(SA)铁植入的氮掺杂多孔碳(Fe -N-C)。得益于单原子铁位点、分级孔隙、定向介孔通道和高导电性,优化后的Fe -N-C在碱性和更具挑战性的酸性介质中均表现出优异的氧还原活性和稳定性,超过了几乎所有非贵金属催化剂和最先进的Pt/C。更具深远意义的是,这种基于MOF的混合配体策略为精确制备高效单原子催化剂开辟了一条新途径。

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