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From Starch to Carbon Materials: Insight into the Cross-Linking Reaction and Its Influence on the Carbonization Process
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2019-07-27 00:00:00 , DOI: 10.1021/acssuschemeng.9b02821 Maoqun Li 1, 2 , Zhihong Bi 1, 2 , Lijing Xie 1 , Guohua Sun 1 , Zhuo Liu 1 , Qingqiang Kong 1 , Xianxian Wei 3 , Cheng-Meng Chen 1
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2019-07-27 00:00:00 , DOI: 10.1021/acssuschemeng.9b02821 Maoqun Li 1, 2 , Zhihong Bi 1, 2 , Lijing Xie 1 , Guohua Sun 1 , Zhuo Liu 1 , Qingqiang Kong 1 , Xianxian Wei 3 , Cheng-Meng Chen 1
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As a renewable biomass product, starch is a fantastic source for preparing various advanced carbon materials. But starch shows poor thermal stability. Its original spherical morphology tends to be disrupted by direct pyrolysis, and the carbon yield is low. Thus, prestabilization by chemical cross-linking is an effective approach to address the above issue. Herein, corn starch was cross-linked by (NH4)2HPO4, followed by carbonization to obtain uniform carbon microspheres. The chemical evolution from starch to carbon was studied systematically using thermogravimetric-mass spectrometry, in situ Fourier transform infrared, X-ray photoelectron spectroscopy, nuclear magnetic resonance, and in situ X-ray diffraction technique. The mechanism of the cross-linking reaction and its influence on the carbonization process were proposed. The introduction of (NH4)2HPO4 promoted the dehydrogenation reaction of starch and further improved its carbonization behaviors. With the increased temperature, more stable heterocyclic aromatic moieties, such as amines, pyridine, pyrrole, and quaternary type N sites, formed in the carbon skeleton, which boosted the growth in cyclization and the size of the polyaromatic units. The further formation of C–O–PO3, C–P–O3, and C2–P–O2 played a critical role in cross-linking of polyaromatic unit fragments into graphitic crystalline, which facilitated the preservation of the natural microspheres morphology. The insights into the thermochemical conversion of starch paved a way for the controllable transformation from organic biomass to inorganic carbon materials, with desired structure and properties.
中文翻译：
从淀粉到碳材料：洞察交联反应及其对碳化过程的影响
作为一种可再生的生物质产品，淀粉是制备各种高级碳材料的绝佳来源。但是淀粉显示出差的热稳定性。其原始的球形形态易于被直接热解破坏，并且碳收率低。因此，通过化学交联进行的预稳定化是解决上述问题的有效方法。在此，玉米淀粉通过（NH 4）2 HPO 4交联。，然后碳化以获得均匀的碳微球。使用热重质谱，原位傅立叶变换红外光谱，X射线光电子能谱，核磁共振和原位X射线衍射技术系统地研究了从淀粉到碳的化学演化。提出了交联反应的机理及其对碳化过程的影响。（NH 4）2 HPO 4的引入促进了淀粉的脱氢反应，进一步改善了淀粉的碳化行为。随着温度的升高，碳骨架中会形成更稳定的杂环芳族部分，例如胺，吡啶，吡咯和N型季铵盐位点，从而促进了环化反应的增长和多环芳烃单元的尺寸。C – O – PO 3，C – P – O 3和C 2 – P – O 2的进一步形成在将多芳族单元片段交联成石墨晶体中起关键作用，这有助于保持天然微球的形态。对淀粉热化学转化的见解为从有机生物质向无机碳材料的可控转化提供了一种具有所需结构和性能的方式。
更新日期：2019-07-27
中文翻译：
从淀粉到碳材料：洞察交联反应及其对碳化过程的影响
作为一种可再生的生物质产品，淀粉是制备各种高级碳材料的绝佳来源。但是淀粉显示出差的热稳定性。其原始的球形形态易于被直接热解破坏，并且碳收率低。因此，通过化学交联进行的预稳定化是解决上述问题的有效方法。在此，玉米淀粉通过（NH 4）2 HPO 4交联。，然后碳化以获得均匀的碳微球。使用热重质谱，原位傅立叶变换红外光谱，X射线光电子能谱，核磁共振和原位X射线衍射技术系统地研究了从淀粉到碳的化学演化。提出了交联反应的机理及其对碳化过程的影响。（NH 4）2 HPO 4的引入促进了淀粉的脱氢反应，进一步改善了淀粉的碳化行为。随着温度的升高，碳骨架中会形成更稳定的杂环芳族部分，例如胺，吡啶，吡咯和N型季铵盐位点，从而促进了环化反应的增长和多环芳烃单元的尺寸。C – O – PO 3，C – P – O 3和C 2 – P – O 2的进一步形成在将多芳族单元片段交联成石墨晶体中起关键作用，这有助于保持天然微球的形态。对淀粉热化学转化的见解为从有机生物质向无机碳材料的可控转化提供了一种具有所需结构和性能的方式。
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