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首页> 外文期刊>Advanced Functional Materials >Hierarchical Cross-Linked Carbon Aerogels with Transition Metal-Nitrogen Sites for Highly Efficient Industrial-Level CO_2 Electroreduction
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Hierarchical Cross-Linked Carbon Aerogels with Transition Metal-Nitrogen Sites for Highly Efficient Industrial-Level CO_2 Electroreduction

机译：具有过渡金属 - 氮气部位的分层交联碳气凝胶，用于高效的工业级CO_2电气

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摘要

Developing highly efficient carbon aerogels (CA) electrocatalysts based on transition metal-nitrogen sites is critical for the CO2 electroreduction reaction (CO2RR). However, simultaneously achieving a high current density and high Faradaic efficiency (FE) still remains a big challenge. Herein, a series of unique 3D hierarchical cross-linked nanostructured CA with metal-nitrogen sites (M-N, M = Ni, Fe, Co, Mn, Cu) is developed for efficient CO2RR. An optimal CA/N-Ni aerogel, featured with unique hierarchical porous structure and highly exposed M-N sites, exhibits an unusual CO2RR activity with a CO FE of 98% at -0.8 V. Notably, an industrial current density of 300 mA cm(-2) with a high FE of 91% is achieved on CA/N-Ni aerogel in a flow-cell reactor, which outperforms almost all previously reported M-N/carbon based catalysts. The CO2RR activity of different CA/N-M aerogels can be arranged as Ni, Fe, Co, Mn, and Cu from high to low. In situ spectroelectrochemistry analyses validate that the rate-determining step in the CO2RR is the formation of *COOH intermediate. A Zn-CO2 battery is further assembled with CA/N-Ni as the cathode, which shows a maximum power density of 0.5 mW cm(-2) and a superior rechargeable stability.
机译：基于过渡金属 - 氮气部位的开发高效碳气（CA）电催化剂对CO 2电氧化碳反应（CO2RR）至关重要。然而，同时实现高电流密度和高法达效率（FE）仍然是一个很大的挑战。在此，开发了一系列具有金属 - 氮位点（M-N，M = Ni，Fe，Co，Mn，Cu）的唯一3D分层交联纳米结构Ca，用于有效CO 2Rr。具有独特的等级多孔结构和高度暴露的Mn位点的最佳CA / N-Ni气凝胶，具有不寻常的CO2RR活性，CO FE为-0.8 V.tax FE，特别是，工业电流密度为300 mA cm（ - 2）在流动细胞反应器中的Ca / N-Ni气凝胶上实现了高Fe的91％，几乎所有先前报道的Mn /碳催化剂均匀。不同Ca / N-M Aerogels的CO 2RR活性可以布置为Ni，Fe，Co，Mn和Cu从高到低。原位光谱电化学分析验证CO2RR中的速率测定步骤是* COOH中间体的形成。 Zn-CO2电池进一步用Ca / N-Ni作为阴极组装，其显示出0.5mm cm（-2）的最大功率密度和可再充电稳定性的优异的可充电稳定性。

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  • 来源
    《Advanced Functional Materials》 |2021年第45期|2104377.1-2104377.10|共10页
  • 作者

    Zhang Yikai; Wang Xinyue; Zheng Sixing; Yang Bin; Li Zhongjian; Lu Jianguo; Zhang Qinghua; Adli Nadia Mohd; Lei Lecheng; Wu Gang; Hou Yang;

  • 作者单位

    Zhejiang Univ Coll Chem & Biol Engn Minist Educ Key Lab Biomass Chem Engn Hangzhou 310027 Peoples R China;

    Zhejiang Univ Coll Chem & Biol Engn Minist Educ Key Lab Biomass Chem Engn Hangzhou 310027 Peoples R China;

    Zhejiang Univ Coll Chem & Biol Engn Minist Educ Key Lab Biomass Chem Engn Hangzhou 310027 Peoples R China;

    Zhejiang Univ Coll Chem & Biol Engn Minist Educ Key Lab Biomass Chem Engn Hangzhou 310027 Peoples R China;

    Zhejiang Univ Coll Chem & Biol Engn Minist Educ Key Lab Biomass Chem Engn Hangzhou 310027 Peoples R China;

    Zhejiang Univ Sch Mat Sci & Engn State Key Lab Silicon Mat Hangzhou 310027 Peoples R China;

    Zhejiang Univ Coll Chem & Biol Engn Minist Educ Key Lab Biomass Chem Engn Hangzhou 310027 Peoples R China;

    Univ Buffalo State Univ New York Dept Chem & Biol Engn Buffalo NY 14260 USA;

    Zhejiang Univ Coll Chem & Biol Engn Minist Educ Key Lab Biomass Chem Engn Hangzhou 310027 Peoples R China|Inst Zhejiang Univ Quzhou Quzhou 324000 Peoples R China;

    Univ Buffalo State Univ New York Dept Chem & Biol Engn Buffalo NY 14260 USA;

    Zhejiang Univ Coll Chem & Biol Engn Minist Educ Key Lab Biomass Chem Engn Hangzhou 310027 Peoples R China|Inst Zhejiang Univ Quzhou Quzhou 324000 Peoples R China;

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  • 关键词

    carbon aerogels; CO; (2) electroreduction; cross-linked nanostructures; isolated M; -N sites; Zn; -CO; (2) batteries;

    机译：碳静电;CO;（2）电荷;交联纳米结构;分离的M;-N位点;Zn;-Co;（2）电池;

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