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含氧三嗪-七嗪杂化结构使多孔 C3N4 纳米片的可见光光催化析氢性能得到极大提升。

Oxygenated Triazine-Heptazine Heterostructure Creates an Enormous Ascension to the Visible Light Photocatalytic Hydrogen Evolution Performance of Porous C N Nanosheets.

机构信息

State Key Laboratory for Organic Electronics and Information Displays & Jiangsu Key Laboratory for Biosensors, Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing University of Posts and Telecommunications, 9 Wenyuan Road, Nanjing, 210023, P. R. China.

Institute of Nanochemistry and Nanobiology, School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, P. R. China.

出版信息

Small. 2023 Jun;19(25):e2301579. doi: 10.1002/smll.202301579. Epub 2023 Mar 15.

DOI:10.1002/smll.202301579
PMID:36919785
Abstract

A highly efficient g-C N photocatalyst is developed by a novel one-pot thermal polymerization method under a salt fog environment generated by heating the aqueous solution of urea and mixed metal salts of NaCl/KCl, namely SF-CN. Thanks to the synergistic effect of the oxygenation and chemical etching of the salt fog, the obtained SF-CN is an oxygenated ultrathin porous carbon nitride with an intermolecular triazine-heptazine heterostructure, meanwhile, shows enlarged specific surface area, greatly enhanced absorption of visible light, narrowed band gap with a lower conduction band, and an increased photocurrent response due to the effective separation of photogenerated holes and electrons, comparing to those of pristine g-C N . The theoretical simulations further reveal that the triazine-heptazine heterostructure possesses better photocatalytic hydrogen evolution (PHE) capability than pure triazine and heptazine carbon nitrides. In turn, SF-CN demonstrates an excellent visible light PHE rate of 18.13 mmol h  g , up to 259.00 times of that of pristine g-C N .

摘要

一种高效的 g-C3N4光催化剂通过在加热尿素和 NaCl/KCl 混合金属盐的水溶液产生的盐雾环境下的新型一锅热聚合方法来制备,即 SF-CN。得益于盐雾的氧化和化学刻蚀的协同作用,所获得的 SF-CN 是一种含氧的超薄多孔碳氮化物,具有分子间的三嗪-六嗪杂化结构,同时具有更大的比表面积、可见光吸收能力大大增强、带隙变窄、导带降低,以及光生空穴和电子的有效分离导致光电流响应增加,与原始的 g-C3N4相比。理论模拟进一步表明,三嗪-六嗪杂化结构具有比纯三嗪和六嗪碳氮化物更好的光催化析氢(PHE)性能。反过来,SF-CN 表现出优异的可见光 PHE 速率为 18.13 mmol h-1 g-1,高达原始 g-C3N4的 259.00 倍。

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