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含氮多孔石墨碳的结构与壳聚糖和 Pluronic P123。

Porous Graphitic Carbons Containing Nitrogen by Structuration of Chitosan with Pluronic P123.

机构信息

Instituto Universitario de Tecnología Química, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas, Av. de los Naranjos s/n, 46022 Valencia, Spain.

出版信息

ACS Appl Mater Interfaces. 2021 Mar 24;13(11):13499-13507. doi: 10.1021/acsami.0c19463. Epub 2021 Mar 11.

Abstract

Using Pluronic P123 as a structure-directing agent and chitosan as a carbon precursor, different porous carbons with remarkable morphologies such as orthohedra or spheres with diametrically opposite holes are obtained. These particles of micrometric size are constituted by the stacking of thin sheets (60 nm) that become increasingly bent in the opposite sense, concave in the upper and convex in the bottom hemispheres, as the chitosan proportion increases. TEM images, after dispersion of the particles by sonication, show that besides micrometric graphene sheets, the material is constituted by nanometric onion-like carbons. The morphology and structure of these porous carbons can be explained based on the ability of Pluronic P123 to undergo self-assembly in aqueous solution due to its amphoteric nature and the filmogenic properties of chitosan to coat Pluronic P123 nanoobjects undergoing structuration and becoming transformed into nitrogen-doped graphitic carbons. XPS analysis reveals the presence of nitrogen in their composition. These porous carbons exhibit a significant CO adsorption capacity of above 3 mmol g under 100 kPa at 273 K attributable to their large specific surface area, ultraporosity, and the presence of basic N sites. In addition, the presence of dopant elements in the graphitic carbons opening the gap is responsible for the photocatalytic activity for H generation in the presence of sacrificial electron donors, reaching a H production of 63 μmol g in 24 h.

摘要

使用 Pluronic P123 作为结构导向剂和壳聚糖作为碳前体,可以获得具有明显形态的不同多孔碳,例如正交多面体或具有相对孔的球体。这些微米级大小的颗粒由薄片(60nm)堆叠而成,随着壳聚糖比例的增加,薄片在相反方向上越来越弯曲,在上半球凹陷,在下半球凸起。TEM 图像显示,在通过超声分散颗粒后,除了微米级的石墨烯片之外,该材料还由纳米洋葱状碳组成。这些多孔碳的形态和结构可以基于 Pluronic P123 由于其两性性质在水溶液中自组装的能力以及壳聚糖成膜性来解释,壳聚糖能够涂覆正在结构化的 Pluronic P123 纳米物体并转化为氮掺杂石墨碳。XPS 分析表明它们的组成中存在氮。这些多孔碳在 273K 时在 100kPa 下的 CO 吸附容量超过 3mmol/g,这归因于其大的比表面积、超多孔性和碱性 N 位的存在。此外,石墨碳中掺杂元素的存在打开了间隙,这是在牺牲电子供体存在下产生 H 的光催化活性的原因,在 24 小时内达到 63μmol/g 的 H 产量。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4f62/8528379/1f66a9ab4600/am0c19463_0009.jpg

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