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研究剥离石墨相氮化碳在溶剂中的分散行为、生物相容性及其作为高效金属催化剂载体的应用。

Investigating the Dispersion Behavior in Solvents, Biocompatibility, and Use as Support for Highly Efficient Metal Catalysts of Exfoliated Graphitic Carbon Nitride.

作者信息

Ayán-Varela M, Villar-Rodil S, Paredes J I, Munuera J M, Pagán A, Lozano-Pérez A A, Cenis J L, Martínez-Alonso A, Tascón J M D

机构信息

Instituto Nacional del Carbón, INCAR-CSIC , Apartado 73, 33080 Oviedo, Spain.

Instituto Murciano de Investigación y Desarrollo Agrario y Alimentario (IMIDA) , Calle Mayor 1, 30150 La Alberca, Spain.

出版信息

ACS Appl Mater Interfaces. 2015 Nov 4;7(43):24032-45. doi: 10.1021/acsami.5b06974. Epub 2015 Oct 26.

DOI:10.1021/acsami.5b06974
PMID:26465228
Abstract

The liquid-phase exfoliation of graphitic carbon nitride (g-C3N4) to afford colloidal dispersions of two-dimensional flakes constitutes an attractive route to facilitate the processing and implementation of this novel material toward different technological applications, but quantitative knowledge about its dispersibility in solvents is lacking. Here, we investigate the dispersion behavior of exfoliated g-C3N4 in a wide range of solvents and evaluate the obtained results on the basis of solvent surface energy and Hildebrand/Hansen solubility parameters. Estimates of the three Hansen parameters for exfoliated g-C3N4 from the experimentally derived data yielded δD ≈ 17.8 MPa(1/2), δP ≈ 10.8 MPa(1/2), and δH ≈ 15.4 MPa(1/2). The relatively high δH value suggested that, contrary to the case of other two-dimensional materials (e.g., graphene or transition metal dichalcogenides), hydrogen-bonding plays a substantial role in the efficient interaction, and thus dispersibility, of exfoliated g-C3N4 with solvents. Such an outcome was attributed to a high density of primary and/or secondary amines in the material, the presence of which was associated with incomplete condensation of the structure. Furthermore, cell proliferation tests carried out on thin films of exfoliated g-C3N4 using murine fibroblasts suggested that this material is highly biocompatible and noncytotoxic. Finally, the exfoliated g-C3N4 flakes were used as supports in the synthesis of Pd nanoparticles, and the resulting hybrids exhibited an exceptional catalytic activity in the reduction of nitroarenes.

摘要

将石墨相氮化碳(g-C3N4)进行液相剥离以获得二维薄片的胶体分散体,为促进这种新型材料在不同技术应用中的加工和应用提供了一条有吸引力的途径,但目前缺乏关于其在溶剂中分散性的定量知识。在此,我们研究了剥离的g-C3N4在多种溶剂中的分散行为,并根据溶剂表面能和希尔德布兰德/汉森溶解度参数对所得结果进行评估。根据实验数据估算出剥离的g-C3N4的三个汉森参数,得到δD≈17.8 MPa(1/2),δP≈10.8 MPa(1/2),δH≈15.4 MPa(1/2)。相对较高的δH值表明,与其他二维材料(如石墨烯或过渡金属二硫属化物)的情况相反,氢键在剥离的g-C3N4与溶剂的有效相互作用以及因此的分散性中起着重要作用。这种结果归因于材料中伯胺和/或仲胺的高密度,其存在与结构的不完全缩合有关。此外,使用鼠成纤维细胞对剥离的g-C3N4薄膜进行的细胞增殖测试表明,这种材料具有高度的生物相容性且无细胞毒性。最后,剥离的g-C3N4薄片被用作合成钯纳米颗粒的载体,所得的杂化物在硝基芳烃的还原反应中表现出优异的催化活性。

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