Ordered Bicontinuous Mesoporous Polymeric Semiconductor Photocatalyst
Ordered Bicontinuous Mesoporous Polymeric Semiconductor Photocatalyst
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有序双连续介孔高分子半导体光催化剂
DOI：
10.1021/acsnano.0c05797
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发表时间：
2020-10-27
期刊：
影响因子：
17.1
通讯作者：
Mai, Yiyong
中科院分区：
文献类型：
--
作者：
Li, Qian;Chen, Chuanshuang;Mai, Yiyong
双连续多孔材料具有三重周期极小表面和三维连通孔结构，在能源、催化等领域具有广泛的应用前景，引起了人们的极大关注。然而，综合这些建议仍然是一个巨大的挑战。在这里，我们展示了一个双连续的多孔有机半导体光催化剂的合成，它涉及到通过溶剂蒸发诱导的自组装的聚苯乙烯-嵌段-聚（环氧乙烷）二嵌段共聚物和正硅酸乙酯，然后由SiO2模板的三聚氰胺单体在真空中的自缩合制备SiO2与移位双金刚石（DD）结构。引人注目的是，所得DD结构的石墨碳氮化物（g-CN）具有平均直径为14 nm的两组3D连续介孔，其提供了131 m2 g-1的高比表面积和2.8 eV的光学带隙。作为一种可见光驱动的光催化剂，双连续介孔g-CN显示出高的催化活性，用于水裂解产生H-2（6831 μ mol g（-1）h（-1）），具有优异的循环稳定性。该研究为构建含有3D连续通道的有序介孔材料提供了一种方案，这有望用于催化应用。
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 SiO2 with a shifted double diamond (DD) structure through solvent evaporation-induced self-assembly of a polystyrene-block-poly(ethylene oxide) diblock copolymer and tetraethyl orthosilicate, followed by SiO2-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(2) g(-1) 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-2 (6831 mu mol g(-1) h(-1)) 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.