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具有基于四嗪分子结构的微孔碳氮化物(C N)用于高效吸附一氧化碳和水。

Microporous Carbon Nitride (C N ) with Tetrazine based Molecular Structure for Efficient Adsorption of CO and Water.

作者信息

Sathish C I, Premkumar S, Chu Xueze, Yu Xiaojiang, Breese Mark B H, Al-Abri Mohammed, Al-Muhtaseb Ala'a H, Karakoti Ajay, Yi Jiabao, Vinu Ajayan

机构信息

Global Innovative Center for Advanced Nanomaterials (GICAN), College of Engineering, Science, and Environment, The University of Newcastle, Callaghan, New South Wales, 2308, Australia.

Singapore Synchrotron Light Source, National University of Singapore, Singapore, 117603, Singapore.

出版信息

Angew Chem Int Ed Engl. 2021 Sep 20;60(39):21242-21249. doi: 10.1002/anie.202108605. Epub 2021 Aug 21.

DOI:10.1002/anie.202108605
PMID:34378296
Abstract

Mesoporous carbon nitrides with C N and C N stoichiometries created a new momentum in the field of organic metal-free semiconductors owing to their unique band structures and high basicity. Here, we report on the preparation of a novel graphitic microporous carbon nitride with a tetrazine based chemical structure and the composition of C N using ultra-stable Y zeolite as the template and aminoguanidine hydrochloride, a high nitrogen-containing molecule, as the CN precursor. Spectroscopic characterization and density functional theory calculations reveal that the prepared material exhibits a new molecular structure, which comprises two tetrazines and one triazine rings in the unit cell and is thermodynamically stable. The resultant carbon nitride shows an outstanding surface area of 130.4 m  g and demonstrates excellent CO adsorption per unit surface area of 47.54 μmol m , which is due to the existence of abundant free NH groups, basic sites and microporosity. The material also exhibits highly selective sensing over water molecules (151.1 mmol g ) and aliphatic hydrocarbons due to its unique microporous structure with a high amount of hydrophilic nitrogen moieties and recognizing ability towards small molecules.

摘要

具有C₃N₄和C₅N₅化学计量比的介孔碳氮化物因其独特的能带结构和高碱性,在无有机金属半导体领域开创了新局面。在此,我们报道了一种基于四嗪化学结构且组成为C₅N₅的新型石墨化微孔碳氮化物的制备方法,该方法以超稳定Y型沸石为模板,以高含氮分子盐酸氨基胍作为CN前驱体。光谱表征和密度泛函理论计算表明,所制备的材料呈现出一种新的分子结构,其晶胞中包含两个四嗪环和一个三嗪环,且具有热力学稳定性。所得的碳氮化物具有130.4 m² g⁻¹的出色比表面积,每单位表面积展现出47.54 μmol m⁻²的优异CO吸附量,这归因于大量游离NH基团、碱性位点和微孔的存在。由于其具有大量亲水性氮部分的独特微孔结构以及对小分子的识别能力,该材料还对水分子(151.1 mmol g⁻¹)和脂肪烃表现出高度选择性传感。

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