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原位二氧化硅干凝胶辅助简便合成具有密集铁氮活性位点的铁氮碳催化剂用于高效氧还原

In-Situ Silica Xerogel Assisted Facile Synthesis of Fe-N-C Catalysts with Dense Fe-N Active Sites for Efficient Oxygen Reduction.

作者信息

Liu Maosong, Wang Lijuan, Zhang Long, Zhao Yiran, Chen Kangmin, Li Yanxiao, Yang Xiaohua, Zhao Long, Sun Shuhui, Zhang Jianming

机构信息

Institute of Quantum and Sustainable Technology (IQST), School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang, 212013, China.

Shanghai Qibao Dwight High School, Shanghai, 201101, China.

出版信息

Small. 2022 Feb;18(7):e2104934. doi: 10.1002/smll.202104934. Epub 2022 Jan 12.

Abstract

In the past decade, atomically dispersed Fe active sites (coordinated with nitrogen) on carbon materials (FeNC) have emerged rapidly as promising single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) to substitute precious group metal (PGM) catalysts, owing to their earth abundance and low cost. Nonetheless, the production of highly active FeNC SACs is largely restricted by material cost, low product yield and difficulty of microstructure design. Herein, the authors demonstrate a facile in-situ xerogel (ISG) assisted synthetic strategy, using cheap materials, to construct FeNC SACs (ISG FeNC). The porous silica xerogel, formed in-situ with the FeNC precursors, encourages the emergence of enormous micropores/mesopores and homogeneous confinement/protection to the precursors during pyrolysis, benefiting to the formation of abundant accessible active sites (27.6 × 10 sites g ). Correspondingly, the ISG FeNC exhibits excellent ORR activity with a half-wave potential (E  = 0.91 V) in alkaline medium. The Zn-air battery assembled using the ISG FeNC SACs as the bifunctional catalyst of air cathode, demonstrates commendable performance with high peak power density of 249.1 mW cm and superior long-term stability (660 cycles with 220 h). This work offers an economic and efficient way to fabricate PGM-free SACs for diverse applications.

摘要

在过去十年中,碳材料上原子分散的铁活性位点(与氮配位)(FeNC)作为用于氧还原反应(ORR)以替代贵金属(PGM)催化剂的有前景的单原子催化剂(SACs)迅速出现,这得益于其丰富的储量和低成本。尽管如此,高活性FeNC SACs的生产在很大程度上受到材料成本、低产品产率和微观结构设计难度的限制。在此,作者展示了一种简便的原位干凝胶(ISG)辅助合成策略,使用廉价材料来构建FeNC SACs(ISG FeNC)。与FeNC前驱体原位形成的多孔二氧化硅干凝胶,在热解过程中促进了大量微孔/介孔的出现以及对前驱体的均匀限制/保护,有利于形成大量可及的活性位点(27.6×10个位点/克)。相应地,ISG FeNC在碱性介质中表现出优异的ORR活性,半波电位(E = 0.91 V)。使用ISG FeNC SACs作为空气阴极的双功能催化剂组装的锌空气电池,表现出令人称赞的性能,高峰功率密度为249.1 mW/cm²,具有出色的长期稳定性(660次循环,共220小时)。这项工作为制造用于各种应用的无PGM SACs提供了一种经济有效的方法。

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