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通过氨基离子液体双模式键合构建3D石墨烯/NH-MIL-125纳米杂化物用于高湿度下的高级乙醛光降解

Construction of 3D-graphene/NH-MIL-125 nanohybrids via amino-ionic liquid dual-mode bonding for advanced acetaldehyde photodegradation under high humidity.

作者信息

Shah Syed Jalil, Luan Xinqi, Yu Xin, Su Weige, Wang Yucheng, Zhao Zhongxing, Zhao Zhenxia

机构信息

School of Chemistry and Chemical Engineering, Key Laboratory of New Low-carbon Green Chemical Technology, Education Department of Guangxi Zhuang Autonomous Region, Guangxi University, Nanning 530004, China; School of Medicine and Health, Harbin Institute of Technology, Harbin, Heilongjiang 150001, China; Zhengzhou Research Institute, Harbin Institute of Technology, Zhengzhou, Henan 450000, China.

School of Chemistry and Chemical Engineering, Key Laboratory of New Low-carbon Green Chemical Technology, Education Department of Guangxi Zhuang Autonomous Region, Guangxi University, Nanning 530004, China.

出版信息

J Colloid Interface Sci. 2024 Jun;663:491-507. doi: 10.1016/j.jcis.2024.02.167. Epub 2024 Feb 24.

Abstract

The development of metal organic framework (MOF)-based π-π conjugated structures capable of effectively transforming HO from humid air to OH radicals for VOCs photodegradation is a significant but difficult task. Herein, an amino-ionic liquid (NH-IL) based dual-mode bridging strategy was proposed to connect 3D-graphene with NH-MIL-125 forming IL-3DGr/NM(Ti) nanohybrids for advanced acetaldehyde photodegradation. The rational integration of these components was responsible for: (1) maintaining π-π conjugated electron transport system; (2) generating abundant coordinatively unsaturated sites and oxygen vacancies; (3) increasing surface area of the nanohybrids. With these attributes, IL-3DGr/NM(Ti) demonstrated enhanced charge separation and transportation electrochemical impedance spectroscopy (EIS): 7-times), acetaldehyde adsorption (22 %), light absorption (bandgap: 1.51 eV). The rapid HO adsorption and photoconversion to OH radicals by IL-3DGr/NM(Ti) enabled it to demonstrate superior CHCHO photodegradation rate under high humidity, surpassing many state-of-the-art photocatalysts by 9 to 187 times under static air conditions and with nearly similar catalyst dosages* (photocatalyst weight and initial acetaldehyde concentration (mg ppm) ratio). Interestingly, the IL-3DGr/NM(Ti) photocatalytic activity was enhanced by increasing RH% up-to 80 %. Besides, the nanohybrids demonstrated tremendous stability, with only a 3.9 % decline observed after 5 consecutive-cycles. This strategy provides new prospects to improve the compatibility of graphene/MOF materials for futuristic photoelectrical applications under high humidity.

摘要

开发能够有效将潮湿空气中的HO转化为OH自由基以用于挥发性有机化合物(VOCs)光降解的基于金属有机框架(MOF)的π-π共轭结构是一项重大但困难的任务。在此,提出了一种基于氨基离子液体(NH-IL)的双模式桥接策略,将3D石墨烯与NH-MIL-125连接起来,形成IL-3DGr/NM(Ti)纳米杂化物,用于高级乙醛光降解。这些组分的合理整合导致:(1)维持π-π共轭电子传输系统;(2)产生大量配位不饱和位点和氧空位;(3)增加纳米杂化物的表面积。具有这些特性,IL-3DGr/NM(Ti)在电荷分离和传输方面表现增强(电化学阻抗谱(EIS):7倍)、乙醛吸附(22%)、光吸收(带隙:1.51 eV)。IL-3DGr/NM(Ti)对HO的快速吸附以及将其光转化为OH自由基,使其在高湿度下表现出优异的CHCHO光降解速率,在静态空气条件下且催化剂用量几乎相同(光催化剂重量与初始乙醛浓度(mg ppm)之比)时,比许多先进的光催化剂高出9至187倍。有趣的是,IL-3DGr/NM(Ti)的光催化活性在相对湿度(RH%)提高到80%时增强。此外,该纳米杂化物表现出极大的稳定性,连续5个循环后仅观察到3.9%的下降。该策略为提高石墨烯/MOF材料在高湿度下未来光电应用的兼容性提供了新的前景。

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