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有序双连续介孔聚合物半导体光催化剂

Ordered Bicontinuous Mesoporous Polymeric Semiconductor Photocatalyst.

作者信息

Li Qian, Chen Chuanshuang, Li Chen, Liu Ruiyi, Bi Shuai, Zhang Pengfei, Zhou Yongfeng, Mai Yiyong

机构信息

School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China.

出版信息

ACS Nano. 2020 Oct 27;14(10):13652-13662. doi: 10.1021/acsnano.0c05797. Epub 2020 Oct 9.

Abstract

Owning triply periodic minimal surfaces and three-dimensional (3D) interconnected pores, bicontinuous porous materials have drawn enormous attention due to their great academic interest and potential applications in many fields including energy and catalysis. However, their synthesis has remained a great challenge. Here, we demonstrate the synthesis of a bicontinuous porous organic semiconductor photocatalyst, which involves the preparation of SiO with a shifted double diamond (DD) structure through solvent evaporation-induced self-assembly of a polystyrene--poly(ethylene oxide) diblock copolymer and tetraethyl orthosilicate, followed by SiO-templated self-condensation of melamine monomers in a vacuum. Strikingly, the resultant DD-structured graphitic carbon nitride (g-CN) possesses two sets of 3D continuous mesopores with a mean diameter of 14 nm, which afford a high specific surface area of 131 m g and an optical band gap of 2.8 eV. Being a visible-light-driven photocatalyst, the bicontinuous mesoporous g-CN exhibits high catalytic activity for water splitting to generate H (6831 μmol g h) with excellent cycling stability. This study provides a protocol for the construction of ordered mesoporous materials containing 3D continuous channels, which holds promise for catalysis applications.

摘要

双连续多孔材料具有三重周期最小表面和三维(3D)互连孔结构,因其具有极大的学术价值以及在包括能源和催化在内的许多领域的潜在应用而备受关注。然而,其合成仍然是一个巨大的挑战。在此,我们展示了一种双连续多孔有机半导体光催化剂的合成方法,该方法包括通过聚苯乙烯 - 聚(环氧乙烷)二嵌段共聚物和正硅酸四乙酯的溶剂蒸发诱导自组装制备具有移位双菱形(DD)结构的SiO,随后在真空中以SiO为模板进行三聚氰胺单体的自缩合。引人注目的是,所得的DD结构石墨相氮化碳(g-CN)具有两组平均直径为14 nm的3D连续介孔,其比表面积高达131 m²/g,光学带隙为2.8 eV。作为一种可见光驱动的光催化剂,双连续介孔g-CN对水分解产生H₂(6831 μmol g⁻¹ h⁻¹)表现出高催化活性,且具有出色的循环稳定性。本研究提供了一种构建包含3D连续通道的有序介孔材料的方案,这为催化应用带来了希望。

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