硅酸盐学报

有机蒙脱石/聚氨酯海绵复合气凝胶去除疏水性有机污染物性能

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何诗雅 ¹^,²^,³ , 刘相君 ¹^,²^,³ , 韦寿淑 ¹^,²^,³ , 陈情泽 ¹^,²^,³ , 朱润良 ¹^,²^,³

硅酸盐学报 | 环境矿物材料专题—研究论文 2024,52(10): 3205-3216

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硅酸盐学报 |环境矿物材料专题—研究论文 2024 , 52 (10) : 3205 -3216

有机蒙脱石/聚氨酯海绵复合气凝胶去除疏水性有机污染物性能

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何诗雅¹^,²^,³, 刘相君¹^,²^,³, 韦寿淑¹^,²^,³, 陈情泽¹^,²^,³, 朱润良¹^,²^,³

作者信息

^1．中国科学院广州地球化学研究所矿物学与成矿学重点实验室/广东省矿物物理与材料开发重点实验室，广州 510640

^2．中国科学院深地科学卓越创新中心，广州 510640

^3．中国科学院大学，北京 100049

通讯作者:

陈情泽（1991—），男，博士，副研究员。

作者简介:

何诗雅（1995—），女，博士研究生；

刘相君（1998—），女，硕士研究生。

Preparation of Organic Montmorillonite/Polyurethane Sponge Composite Aerogel for Removal of Hydrophobic Organic Contaminants

Shiya HE¹^,²^,³, Xiangjun LIU¹^,²^,³, Shoushu WEI¹^,²^,³, Qingze CHEN¹^,²^,³, Runliang ZHU¹^,²^,³

Affiliations

^1.Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, CAS Key Laboratory of Mineralogy and Metallogeny/Guangdong Provincial Key Laboratory of Mineral Physics and Material, Guangzhou 510640, China

^2.CAS Center for Excellence in Deep Earth Science, Guangzhou 510640, China

^3.University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding Author:

CHEN Qingze (1991-), male, Ph.D., Associate Professor. E-mail: chenqingze@gig.ac.cn

HE Shiya (1995-), female, Doctoral candidate; E-mail: heshiya@gig.ac.cn;

LIU Xiangjun (1998-), female, Master candidate. 18062441976@139.com.

出版时间: 2024-10-20 doi: 10.14062/j.issn.0454-5648.20240155

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摘要

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疏水性有机污染物对生态系统和人类健康造成了严重危害，亟需开发低成本、高效、环保及可再生的吸附剂用于去除疏水性有机污染物。通过超声溶胀和冷冻干燥法制得密度低（34.61 mg/cm³）、疏水性强和可燃性低的有机蒙脱石/聚氨酯海绵复合气凝胶。对该复合气凝胶的形貌和结构进行了分析，并探究了其对疏水性有机污染物、油和有机溶剂的吸附/吸收能力。结果表明：有机蒙脱石/聚氨酯海绵复合气凝胶对苯蒸汽的静态吸附量可达682.3 mg/g，对溶液中双酚A和硝基苯的吸附量分别为339.8 mg/g和137.0 mg/g，对不同油和有机溶剂的吸收量为20.8~37.0 g/g，且具有良好的可重复利用性。此外，有机蒙脱石/聚氨酯海绵复合气凝胶对实际污水中的有机物也有较好的吸收性能（7.12 g/g），且易于回收利用，有望作为一种高效的蒙脱石基吸附材料应用于污染控制领域。

关键词

蒙脱石 / 气凝胶 / 吸附 / 有机污染物 / 油/水分离

Abstract

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Introduction

Hydrophobic organic pollutants in industrial wastewater and oil spillage have attracted wide attention. It is thus important to develop a variety of adsorbents like activated carbon, biochar, zeolite, graphene, etc.. However, carbon-based porous materials exhibit poor thermal stability and flammability, having secure risks during high-temperature applications and thermal regeneration processes. Silicon-based porous materials like zeolite are complex to prepare and difficult to effectively remove multiple organic pollutants simultaneously. Montmorillonite-based adsorbents become popular due to their low cost and environmental friendliness. However, montmorillonite as a powder has challenges in practical applications such as clogging, leakage, and recovery difficulties. It is thus effective in converting montmorillonite into fixed-form aerogel materials.

Polyurethane sponge (PU) as an ideal substrate for developing porous aerogels can enhance the mechanical properties of the adsorbents due to its biodegradability, affordability, low density, and customizable dimensions. In this paper, low-density, recyclable, and cost-effective organic montmorillonite/polyurethane sponge composite aerogels were prepared via ultrasonic swelling and freeze-drying. The composite aerogel was evaluated for its adsorption/absorption capabilities towards benzene, bisphenol A, nitrobenzene, oils, and organic solvents. In addition, the reusability and flammability characteristics of the aerogel were also analyzed.

Methods

An organic montmorillonite (i.e., C16Mnt) was prepared with cetyltrimethylammonium bromide to modify montmorillonite. 1 g C16Mnt was added to 20 mL organic solvent (the mass ratio of cyclohexane to tertiary butanol is 9∶1) to prepare a suspension C16Mnt. Chitosan sol was then introduced into the suspension C16Mnt and agitated in a water bath at 50 ℃ for 3 h, yielding a homogeneous sol. Subsequently, PU was immersed in the sol for 5 min to ensure a complete absorption. The sol-loaded PU was subsequently aged at 25 ℃ for 12 h, facilitating the transformation of the sol into a gel. The organic montmorillonite/polyurethane sponge composite aerogel (i.e., PU/CS-C16Mnt) was fabricated via freezing the gel in liquid nitrogen for 10 min and subsequently freeze-drying for 48 h. The composite aerogels, differing in densities (PU25 and PU35), were denoted as PU25/CS-C16Mnt and PU35/CS-C16Mnt, respectively.

Results and discussion

PU has a three-dimensional porous network structure and a smooth surface on its skeleton. The pore structure of PU undergoes a significant change after loading with CS-C16Mnt. The pores are filled with numerous organic montmorillonite clusters, resulting in a rougher surface, which is favorable for enhancing the adsorption performance. The incorporation of CS-C16Mnt also improves the hydrophobicity of PU. Furthermore, the infrared spectroscopic analysis reveals that CS-C16Mnt is loaded onto the PU skeleton through covalent bonds and hydrogen bonds formed between PU and CS-C16Mnt.

The PU/CS-C16Mnt exhibits exceptional adsorption capabilities for organic pollutants, based primarily on organic distribution and pore-filling mechanisms. The adsorption results indicate that PU25/CS-C16Mnt has the maximum static adsorption performance for benzene (i.e., 682.3 mg/g). This superior performance can be attributed to the intense interactions with the benzene molecules and C16Mnt, as well as the presence of an abundance of macropores. Besides, PU25/CS-C16Mnt has excellent adsorption properties for bisphenol A and nitrobenzene, achieving adsorption capacities of 339.8 mg/g and 137.0 mg/g, respectively. The infrared spectroscopic results show that O―H and N―H in PU25/CS-C16Mnt participate in the adsorption process. The cyclic adsorption results show that the adsorption capacity of PU25/CS-C16Mnt for bisphenol A decreases from 208.4 mg/g to 154.7 mg/g, and the adsorption capacity of nitrobenzene decreases from 57.9 mg/g to 41.6 mg/g, which is still higher than that of original PU25.

Furthermore, PU25/CS-C16Mnt has good hydrophobicity and lipophilicity, which can selectively absorb oil and organic solvents with the maximum absorption capacity (i.e., 20.8~37.0 g/g) of xylene, gasoline, liquid paraffin, dimethyl silicone oil and carbon tetrachloride. After 10 repeated experiments, the absorption capacity can still maintain 82.8% of the first absorption capacity. Also, PU25/CS-C16Mnt has a good absorption performance (i.e., 7.12 g/g) for grease in actual sewage, and it is easily recyclable. The combustion behavior of PU25/CS-C16Mnt reveals that the incorporation of organic montmorillonite significantly enhances the flammable retardancy of pure PU.

Conclusions

Organic montmorillonite/polyurethane sponge composite aerogel with low-density (i.e., 34.61 mg/cm³), highly hydrophobic and low flammability was synthesized via ultrasonic swelling and freeze-drying. The montmorillonite/polyurethane sponge composite aerogel exhibited exceptional adsorption capabilities for organic pollutants, relying primarily on organic distribution and pore-filling mechanisms. The aerogel demonstrated a static adsorption capacity of 682.3 mg/g for benzene vapor and respective adsorption capacities of 339.8 mg/g for bisphenol A and 137.0 mg/g for nitrobenzene. The absorption capacity for various oils and organic solvents ranged from 20.8-37.0 g/g, with the excellent reusability. Furthermore, montmorillonite/polyurethane sponge composite aerogel exhibited a good adsorption/absorption performance (i.e., 7.12 g/g) for organic contaminants in actual wastewater. This aerogel could be used as a promising montmorillonite-based adsorption material for the treatment of organic pollution.

Key words

montmorillonite / aerogel / adsorption / organic contaminants / oil/water separation

引用本文

何诗雅, 刘相君, 韦寿淑, 陈情泽, 朱润良. 有机蒙脱石/聚氨酯海绵复合气凝胶去除疏水性有机污染物性能. 硅酸盐学报, 2024 , 52 (10) : 3205 -3216 . DOI: 10.14062/j.issn.0454-5648.20240155

Shiya HE, Xiangjun LIU, Shoushu WEI, Qingze CHEN, Runliang ZHU. Preparation of Organic Montmorillonite/Polyurethane Sponge Composite Aerogel for Removal of Hydrophobic Organic Contaminants[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (10) : 3205 -3216 . DOI: 10.14062/j.issn.0454-5648.20240155

基金

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中国科学院青年创新促进会项目(2020347)
广东省自然科学基金杰出青年基金项(2023B1515020006)
广东省科技计划项目(2023B1212060048)

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2024年第52卷第10期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240155

接收时间：2024-02-28
首发时间：2026-10-22
出版时间：2024-10-20

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收稿日期：2024-02-28
修回日期：2024-04-22

基金

中国科学院青年创新促进会项目(2020347)

广东省自然科学基金杰出青年基金项(2023B1515020006)

广东省科技计划项目(2023B1212060048)

作者信息

^1．中国科学院广州地球化学研究所矿物学与成矿学重点实验室/广东省矿物物理与材料开发重点实验室，广州 510640

^2．中国科学院深地科学卓越创新中心，广州 510640

^3．中国科学院大学，北京 100049

通讯作者:

陈情泽（1991—），男，博士，副研究员。

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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