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基于MOF-808/RGO的三维宏观气凝胶的简便合成用于增强光还原CO。

Facile synthesis of MOF-808/RGO-based 3D macroscopic aerogel for enhanced photoreduction CO.

作者信息

Song Mingming, Li Jinze, Xu Mengyang, Xu Zenghui, Song Xianghai, Liu Xin, Zhang Jisheng, Yang Yangyang, Xie Xinmin, Zhou Weiqiang, Huo Pengwei

机构信息

Institute of Green Chemistry and Chemical Technology, School of Chemistry & Chemical Engineering, Jiangsu University, Zhenjiang 212013, China.

China Construction Power and Environment Engineering Co., Ltd., Nanjing 210012, China; China Construction Eco-environmental Protection Technology CO., LTD., Suzhou 215124, China.

出版信息

J Colloid Interface Sci. 2024 Aug 15;668:471-483. doi: 10.1016/j.jcis.2024.04.195. Epub 2024 Apr 28.

Abstract

Three-dimensional (3D) macroscopic aerogels have emerged as a critical component in the realm of photocatalysis. Maximizing the integration of materials can result in enhanced efficiency and selectivity in photocatalytic processes. In this investigation, we fabricated MOF-808/reduced graphene oxide (RGO) 3D macroscopic aerogel composite materials employing the techniques of hydrothermal synthesis and freeze-drying. The results revealed that the macroscopic aerogel material exhibited the highest performance in CO reduction to CO, particularly when the concentration of RGO was maintained at 5 mg mL. In addition, we synthesized powder materials of MR-5 composite photocatalysts and conducted a comparative analysis in terms of photocatalytic CO reduction performance and electron transfer efficiency. The results showthat the macroscopic aerogel material boasts a high specific surface area, an abundant internal pore structure, and increased active sites. These attributes collectively enhance light energy utilization, and electron transfer rates, thereby, improving photothermal and photoelectric conversion efficiencies. Furthermore, we conducted in-situ FT-IR measurements and found that the M/R-5 aerogel exhibited the best CO adsorption capacity under a CO flow rate of 10 mL min. The density functional theory results demonstrate the correlation between the formation pathway of the product and the charge transfer pathway. This study provides useful ideas for realizing photocatalytic CO reduction of macroscopic aerogel materials in gas-solid reaction mode.

摘要

三维(3D)宏观气凝胶已成为光催化领域的关键组成部分。最大化材料的整合可提高光催化过程的效率和选择性。在本研究中,我们采用水热合成和冷冻干燥技术制备了MOF-808/还原氧化石墨烯(RGO)三维宏观气凝胶复合材料。结果表明,宏观气凝胶材料在将CO还原为CO方面表现出最高性能,特别是当RGO浓度保持在5 mg/mL时。此外,我们合成了MR-5复合光催化剂的粉末材料,并对光催化CO还原性能和电子转移效率进行了对比分析。结果表明,宏观气凝胶材料具有高比表面积、丰富的内部孔隙结构和更多的活性位点。这些特性共同提高了光能利用率和电子转移速率,从而提高了光热和光电转换效率。此外,我们进行了原位傅里叶变换红外光谱测量,发现M/R-5气凝胶在CO流速为10 mL/min时表现出最佳的CO吸附能力。密度泛函理论结果证明了产物形成途径与电荷转移途径之间的相关性。本研究为实现气固反应模式下宏观气凝胶材料的光催化CO还原提供了有益思路。

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