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高温合成对石墨相氮化碳结构及其产氢能力的影响。

Influence of High Temperature Synthesis on the Structure of Graphitic Carbon Nitride and Its Hydrogen Generation Ability.

作者信息

Alwin Emilia, Kočí Kamila, Wojcieszak Robert, Zieliński Michał, Edelmannová Miroslava, Pietrowski Mariusz

机构信息

Faculty of Chemistry, Adam Mickiewicz University in Poznań, Uniwersytetu Poznańskiego 8, 61-614 Poznań, Poland.

Univ. Lille, CNRS, Centrale Lille, Univ. Artois, UMR 8181-UCCS-Unité de Catalyse et Chimie du Solide, F-59000 Lille, France.

出版信息

Materials (Basel). 2020 Jun 17;13(12):2756. doi: 10.3390/ma13122756.

DOI:10.3390/ma13122756
PMID:32560554
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7344968/
Abstract

Graphitic carbon nitride (g-CN) was obtained by thermal polymerization of dicyandiamide, thiourea or melamine at high temperatures (550 and 600 °C), using different heating rates (2 or 10 °C min) and synthesis times (0 or 4 h). The effects of the synthesis conditions and type of the precursor on the efficiency of g-CN were studied. The most efficient was the synthesis from dicyandiamide, 53%, while the efficiency in the process of synthesis from melamine and thiourea were much smaller, 26% and 11%, respectively. On the basis of the results provided by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), infrared spectroscopy (FTIR), ultraviolet-visible spectroscopy (UV-vis), thermogravimetric analysis (TGA), elemental analysis (EA), the best precursor and the optimum conditions of synthesis of g-CN were identified to get the product of the most stable structure, the highest degree of ordering and condensation of structure and finally the highest photocatalytic activity. It was found that as the proton concentration decreased and the degree of condensation increased, the hydrogen yields during the photocatalytic decomposition of water-methanol solution were significantly enhanced. The generation of hydrogen was 1200 µmol g and the selectivity towards hydrogen of more than 98%.

摘要

通过在高温（550和600°C）下热聚合双氰胺、硫脲或三聚氰胺来制备石墨相氮化碳（g-CN），采用不同的加热速率（2或10°C/min）和合成时间（0或4小时）。研究了合成条件和前驱体类型对g-CN效率的影响。最有效的是由双氰胺合成，效率为53%，而由三聚氰胺和硫脲合成过程中的效率要小得多，分别为26%和11%。基于X射线衍射（XRD）、X射线光电子能谱（XPS）、红外光谱（FTIR）、紫外可见光谱（UV-vis）、热重分析（TGA）、元素分析（EA）提供的结果，确定了g-CN的最佳前驱体和最佳合成条件，以获得结构最稳定、结构有序度和缩合度最高且最终光催化活性最高的产物。发现随着质子浓度降低和缩合度增加，水-甲醇溶液光催化分解过程中的氢气产率显著提高。氢气生成量为1200 μmol/g，对氢气的选择性超过98%。

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