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通过超快氨等离子体浸没改性调控石墨相氮化碳表面氨基并进行结构工程以增强光催化活性

Surface Amino Group Regulation and Structural Engineering of Graphitic Carbon Nitride with Enhanced Photocatalytic Activity by Ultrafast Ammonia Plasma Immersion Modification.

作者信息

Kang Shifei, He Maofen, Chen Mengya, Liu Yanfei, Wang Yuting, Wang Yangang, Dong Mingdong, Chang Xijiang, Cui Lifeng

机构信息

Department of Environmental Science and Engineering , University of Shanghai for Science and Technology , Shanghai 200093 , P.R. China.

Interdisciplinary Nanoscience Center (iNANO) , Aarhus University , DK-8000 Aarhus , Denmark.

出版信息

ACS Appl Mater Interfaces. 2019 Apr 24;11(16):14952-14959. doi: 10.1021/acsami.9b01068. Epub 2019 Apr 16.

Abstract

Surface amino group regulation and structural engineering of graphitic carbon nitride (g-CN) for better catalytic activity have increasingly become a focus of academia and industry. In this work, the ammonia plasma produced by a microwave surface wave plasma generator was developed as a facile source to achieve fast, controllable surface modification, and structural engineering of g-CN by ultrafast plasma treatment in minutes, thus enhancing photocatalytic performance of g-CN. The morphology, surface hydrophilicity, optical absorption properties, and states of C-N bonds were investigated to determine the effect of plasma immersion modification on the g-CN catalyst. The structure and photoelectric features of the plasma-modified samples were characterized by X-ray diffractometry, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and electrochemical impedance spectroscopy. The results indicate that the ammonia plasma-treated g-CN-NH exhibits an ultrathin nanosheet structure, enriched amino groups, and an ideal molecular structure, a narrower band gap (2.35 eV), extended light-harvesting edges (560 nm), and enhanced electron transport ability. The remarkably enhanced photocatalytic activity demonstrated in the photoreduction and detoxification of hexavalent chromium (Cr(VI)) can be ascribed to the optimization of the structural and photoelectric properties induced by the unique ammonia plasma treatment. The effective and ultrafast approach developed in this work is promising in the surface amino group regulation and structural engineering of various functional materials.

摘要

对石墨相氮化碳(g-CN)进行表面氨基调控和结构工程以提高催化活性,日益成为学术界和工业界的关注焦点。在本工作中,利用微波表面波等离子体发生器产生的氨等离子体,作为一种简便的源,通过在数分钟内进行超快等离子体处理,实现对g-CN的快速、可控表面改性和结构工程,从而提高g-CN的光催化性能。研究了其形貌、表面亲水性、光吸收特性以及C-N键的状态,以确定等离子体浸没改性对g-CN催化剂的影响。通过X射线衍射、傅里叶变换红外光谱、X射线光电子能谱和电化学阻抗谱对等离子体改性样品的结构和光电特性进行了表征。结果表明,氨等离子体处理的g-CN-NH呈现出超薄纳米片结构、富集的氨基和理想的分子结构,带隙更窄(2.35 eV)、光捕获边缘扩展(560 nm)且电子传输能力增强。在六价铬(Cr(VI))的光还原和解毒中表现出的显著增强的光催化活性,可归因于独特的氨等离子体处理诱导的结构和光电性能的优化。本工作中开发的有效且超快的方法,在各种功能材料的表面氨基调控和结构工程方面具有广阔前景。

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