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具有增强电荷转移的石墨相氮化碳六方玫瑰花结的合成,用于增强可见光光催化析氢和过氧化氢生成。

Synthesis of hexagonal rosettes of g-CN with boosted charge transfer for the enhanced visible-light photocatalytic hydrogen evolution and hydrogen peroxide production.

作者信息

Mahvelati-Shamsabadi Tahereh, Fattahimoghaddam Hossein, Lee Byeong-Kyu, Bae Sanghyun, Ryu Jungki

机构信息

DeparFVtment of Civil and Environmental Engineering, University of Ulsan, Daehak-ro 93, Nam-gu, Ulsan 44610, Republic of Korea.

DeparFVtment of Civil and Environmental Engineering, University of Ulsan, Daehak-ro 93, Nam-gu, Ulsan 44610, Republic of Korea.

出版信息

J Colloid Interface Sci. 2021 Sep;597:345-360. doi: 10.1016/j.jcis.2021.04.019. Epub 2021 Apr 8.

DOI:10.1016/j.jcis.2021.04.019
PMID:33892420
Abstract

Photocatalytic sustainable fuel production attracted extensive attention because of the urgent need of the society to shift from fossil fuels to solar fuels. Herein, the synthesis of hexagonal rosettes of g-CN with an efficient performance toward hydrogen evolution and hydrogen peroxide production as the two kinds of solar fuels were reported. The hexagonal rosettes of g-CN were simply fabricated via controlled solid-state polymerization of three-dimensional hexagonal rosettes of cyanuric acid-melamine adduct at 500 °C. The hexagonal rosettes of g-CN showed an amorphous nature with an extremely high surface area of 400 m g. Also, the as-obtained catalyst demonstrated remarkable photocatalytic activity in hydrogen production of 1285 μmol g h and hydrogen peroxide production of 150 μmol g h. The mechanism for the polymerization process of the cyanuric acid-melamine (CM) complex to hexagonal rosettes of g-CN was thoroughly described employing electron microscopy tools. This study identified that the CM complex condensation is accomplished via a dehydration process by producing a highly condensed and active structure of g-CN, which is different from the previously reported condensation mechanism of the melamine and its derivatives performed through a deamination process.

摘要

由于社会迫切需要从化石燃料转向太阳能燃料,光催化可持续燃料生产引起了广泛关注。在此,报道了具有高效产氢和产过氧化氢性能的二维石墨相氮化碳(g-CN)六方玫瑰花结的合成,这两种物质都属于太阳能燃料。g-CN六方玫瑰花结通过三聚氰胺-三聚氰酸加合物的三维六方玫瑰花结在500℃下的可控固态聚合简单制备而成。g-CN六方玫瑰花结呈现无定形性质,具有400 m²/g的极高比表面积。此外,所制备的催化剂在产氢量为1285 μmol g⁻¹ h⁻¹和产过氧化氢量为150 μmol g⁻¹ h⁻¹方面表现出显著的光催化活性。利用电子显微镜工具详细描述了三聚氰胺-三聚氰酸(CM)复合物聚合成g-CN六方玫瑰花结的过程机理。该研究确定,CM复合物的缩合是通过脱水过程完成的,生成了高度缩合且具有活性的g-CN结构,这与之前报道的三聚氰胺及其衍生物通过脱氨基过程进行的缩合机理不同。

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