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Three-dimensional graphene oxide cross-linked by benzidine as an efficient metal-free photocatalyst for hydrogen evolution

机译:通过苯并丁片交联的三维石墨烯氧化物作为氢气进化的有效的金属光催化剂

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The use of low-cost photocatalysts to split water into H _(2) fuel via solar energy is highly desirable for the production of clean energy and a sustainable society. Here three-dimensional graphene oxide (3DG) porous materials were prepared by cross-linking graphene oxide (GO) sheets using aromatic diamines (benzidine, 2,2′-dimethyl-4,4′-biphenyldiamine, 4,4′-diaminodiphenylmethane) that reacted with the carboxyl groups of the GO sheets at room temperature. The prepared 3DG porous materials were used as efficient metal-free photocatalysts for the production of H _(2) via water splitting under full-spectrum light, where the photocatalytic activity was highly dependent on the cross-linker and the 3DG reduction level. It was also found that the 3DG prepared with benzidine as the linker demonstrated a significantly higher H _(2) evolution rate than the 3DGs prepared using 2,2′-dimethyl-4,4′-biphenyldiamine and 4,4′-diaminodiphenylmethane as the cross-linkers. The photoactivity was further tuned by varying the mass ratio of GO to benzidine. Among the prepared 3DG materials, 3DG-3, with an intermediate C/O ratio of 1.84, exhibited the highest H _(2) production rate (690 μmol g ~(?1) h ~(?1) ), which was significantly higher than the two-dimensional GO (45 μmol g ~(?1) h ~(?1) ) and the noncovalent 3DG synthesized by a hydrothermal method (128 μmol g ~(?1) h ~(?1) ). Moreover, this study revealed that the 3DG photocatalytic performance was favored by effective charge separation, while it could be further tuned by changing the reduction level. In addition, these results could prompt the preparation of other 3D materials and the application of new types of photocatalysts for H _(2) evolution.
机译:使用低成本的光催化剂通过太阳能将水分成H _(2)燃料,对于清洁能源和可持续社会来说,非常适合。这里通过使用芳族二胺交联石墨烯氧化物(GO)片(苯并胺,2,2'-二甲基-4,4'-Biphyldiam,4,4'-二氨基二苯基甲烷来制备三维石墨烯氧化物(3DG)多孔材料。与室温下的甲板的羧基反应。将制备的3DG多孔材料用作高效的金属光催化剂,通过在全谱光下通过水分解生产H _(2),其中光催化活性高度依赖于交联剂和3DG还原水平。还发现,用苯并丁作为接头制备的3DG显示出比使用2,2'-二甲基-4,4'-Biphyldinine和4,4'-二氨基二苯基甲烷制备的3DG的显着更高的H _(2)进化率交联剂。通过改变去苯胺的质量比进一步调整光脱离。在制备的3DG材料中,具有1.84的中间C / O比的3DG-3表现出最高的H _(2)生产率(690μmolg〜(α1)H〜(?1)),这显着高于二维GO(45μmolg〜(α1)H〜(α1))和通过水热法合成的非共价3DG(128μmolg〜(α1)h〜(α1))。此外,该研究表明,3DG光催化性能受到有效电荷分离的青睐,而可以通过改变还原水平进一步调整。此外,这些结果可以促使其他3D材料的制备以及适用于H _(2)进化的新型光催化剂。

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