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Direct Heating Amino Acids with Silica: A Universal Solvent-Free Assembly Approach to Highly Nitrogen-Doped Mesoporous Carbon Materials

机译:与二氧化硅直接加热氨基酸:高氮掺杂的介孔碳材料的通用无溶剂组装方法

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摘要

A general solvent-free assembly approach via directly heating amino acid and mesoporous silica mixtures is developed for the synthesis of a family of highly nitrogen-doped mesoporous carbons. Amino acids have been used as the sole precursors for templating synthesis of a series of ordered mesoporous carbons. During heating, amino acids are melted and strongly interact with silica, leading to effective loading and improved carbon yields (up to approximate to 25 wt%), thus to successful structure replication and nitrogendoping. Unique solvent-free structure assembly mechanisms are proposed and elucidated semi-quantitatively by using two affinity scales. Significantly high nitrogen-doping levels are achieved, up to 9.4 (16.0) wt% via carbonization at 900 (700) degrees C. The diverse types of amino acids, their variable interactions with silica and different pyrolytic behaviors lead to nitrogen-doped mesoporous carbons with tunable surface areas (700-1400 m(2) g(-1)), pore volumes (0.9-2.5 cm(3) g(-1)), pore sizes (4.3-10 nm), and particle sizes from a single template. As demonstrations, the typical nitrogen-doped carbons show good performance in CO2 capture with high CO2/N-2 selectivities up to approximate to 48. Moreover, they show attractive performance for oxygen reduction reaction, with an onset and a half-wave potential of approximate to 0.06 and 0.14 V (vs Ag/AgCl).
机译:通过直接加热氨基酸和中孔二氧化硅混合物的通用无溶剂组装方法被开发用于合成高氮掺杂的中孔碳族。氨基酸已用作模板合成一系列有序介孔碳的唯一前体。在加热过程中,氨基酸熔化并与二氧化硅强烈相互作用,从而导致有效负载并提高了碳收率(高达约25 wt%),从而成功实现了结构复制和氮掺杂。提出了独特的无溶剂结构组装机理,并通过使用两个亲和度标度半定量地阐明了该机理。通过在900(700)摄氏度下进行碳化,可以实现高达9.4(16.0)wt%的高氮掺杂水平。多种类型的氨基酸,它们与二氧化硅的可变相互作用以及不同的热解行为会导致氮掺杂的中孔碳具有可调的表面积(700-1400 m(2)g(-1)),孔体积(0.9-2.5 cm(3)g(-1)),孔径(4.3-10 nm)和来自单个模板。作为演示,典型的氮掺杂碳在CO2捕获中表现出良好的性能,并具有高达约48的高CO2 / N-2选择性。此外,它们在氧还原反应方面表现出诱人的性能,其起伏和半波电势为大约为0.06和0.14 V(vs Ag / AgCl)。

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  • 来源
    《Advanced Functional Materials》 |2016年第36期|6649-6661|共13页
  • 作者单位

    Soochow Univ, Coll Chem Chem Engn & Mat Sci, Sch Chem & Environm Engn, Suzhou Key Lab Green Chem Engn, Suzhou 215123, Jiangsu, Peoples R China;

    Soochow Univ, Coll Chem Chem Engn & Mat Sci, Sch Chem & Environm Engn, Suzhou Key Lab Green Chem Engn, Suzhou 215123, Jiangsu, Peoples R China;

    Soochow Univ, Coll Chem Chem Engn & Mat Sci, Sch Chem & Environm Engn, Suzhou Key Lab Green Chem Engn, Suzhou 215123, Jiangsu, Peoples R China;

    Soochow Univ, Coll Chem Chem Engn & Mat Sci, Sch Chem & Environm Engn, Suzhou Key Lab Green Chem Engn, Suzhou 215123, Jiangsu, Peoples R China;

    Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China|Fudan Univ, Adv Mat Lab, Shanghai 200433, Peoples R China;

    Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China|Fudan Univ, Adv Mat Lab, Shanghai 200433, Peoples R China;

    Soochow Univ, Coll Chem Chem Engn & Mat Sci, Sch Chem & Environm Engn, Suzhou Key Lab Green Chem Engn, Suzhou 215123, Jiangsu, Peoples R China;

    Soochow Univ, Coll Chem Chem Engn & Mat Sci, Sch Chem & Environm Engn, Suzhou Key Lab Green Chem Engn, Suzhou 215123, Jiangsu, Peoples R China;

    Soochow Univ, Coll Chem Chem Engn & Mat Sci, Sch Chem & Environm Engn, Suzhou Key Lab Green Chem Engn, Suzhou 215123, Jiangsu, Peoples R China;

    Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China|Fudan Univ, Adv Mat Lab, Shanghai 200433, Peoples R China|Monash Univ, Dept Chem Engn, Clayton, Vic 3800, Australia;

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