Preparation of carbon nanotube-graphene composite aerogel and evaluation of photothermal assisted oil absorption performance

doi:10.16085/j.issn.1000-6613.2023-1745

Abstract

Abstract:

Graphene oxide (GO) and carboxylated multi-walled carbon nanotubes (MWCNTs/COOH) were used as raw materials for the preparation of Pickering emulsion, which was used as a soft template for the synthesis of carbon nanotubes/graphene composite aerogel (CNTs/STRGA) with "droplet-like" pore structure and large pore volume. The photothermal conversion performance of the materials was improved by introducing MWCNTs/COOH. By adjusting the mass ratio between GO and MWCNTs/COOH, oil/water ratio and hydrothermal reduction time, a series of CNTs/STRGAs with different properties were obtained. The prepared materials were characterized using scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), Raman spectrometer and Fourier transform infrared spectrometer (FTIR) to analyze their internal structure and chemical properties. A UV visible near-infrared spectrophotometer and a microcomputer controlled electronic universal testing machine were used to evaluate the light absorbance and mechanical properties of materials. The results showed that MWCNTs/COOH could significantly improve the light absorbance (95.2%) and photo-thermal conversion performance of the material, and the surface of the material could be heated to 130℃ under 1 sun illumination. The photothermal oil adsorption rate of the material was significantly enhanced, 6.88g/(g·min), and its adsorption capacity reached 130.66g/g.

Key words: Pickering emulsion, graphene, aerogel, carbon nanotubes, photothermal-adsorption

摘要：

以氧化石墨烯（GO）、羧基化多壁碳纳米管（MWCNTs/COOH）为原料制备Pickering乳液，并以其为软模板合成具有“液滴状”孔道结构和大孔隙体积的碳纳米管/石墨烯复合气凝胶（CNTs/STRGA）。通过引入MWCNTs/COOH的方式，提高材料的光热转换性能。调整GO与MWCNTs/COOH的质量比、油水比、水热还原时间，得到一系列不同性质的CNTs/STRGAs。通过扫描电子显微镜（SEM）、X射线光电子能谱（XPS）、拉曼光谱仪（Raman）和傅里叶变换红外光谱仪（FTIR）对所制备的材料进行表征。采用紫外-可见-近红外分光光度计、微机控制电子万能试验机评价材料的吸光能力和机械性能。结果表明，MWCNTs/COOH能显著提高材料的吸光度（95.2%）和光热转换性能，材料上表面通过光热转换可升温至130℃，材料的光热-吸油速率会明显提升，可达6.88g/(g·min)，其吸附容量可达130.66g/g。

关键词: Pickering乳液, 石墨烯, 气凝胶, 碳纳米管, 光热-吸附

CLC Number:

TQ013.2

GUO Qilin, GUO Shi, ZHANG Yingbo, PAN Yiyong, CHEN Zhikang, CHEN Shuang, LIU Hui’e, SHEN Qi, GUO Rongrong. Preparation of carbon nanotube-graphene composite aerogel and evaluation of photothermal assisted oil absorption performance[J]. Chemical Industry and Engineering Progress, 2024, 43(11): 6317-6326.

郭启麟, 郭适, 张瀛博, 潘宜勇, 陈志康, 陈爽, 刘会娥, 申琦, 郭蓉蓉. 碳纳米管/石墨烯复合气凝胶的制备与光热辅助吸油性能评价[J]. 化工进展, 2024, 43(11): 6317-6326.

Figures/Tables 13

References 33

1	OUYANG Yuqing, SONG Linhua, ZHAO Xiaodong, et al. 3D flexible superhydrophobic polyphosphazene coated melamine sponge for oil-water separation[J]. Separation and Purification Technology, 2023, 306: 122600.
2	ZHANG Guoxing, SUN Huixuan, GONG Qirui, et al. Preparation and modification of antibacterial polyurethane foam for oil-water separation[J]. Journal of Materials Research, 2023, 38(10): 2701-2712.
3	BAI Xiangge, YUAN Zichao, LU Chenguang, et al. Recent advances in superwetting materials for separation of oil/water mixtures[J]. Nanoscale, 2023, 15(11): 5139-5157.
4	YAN Xi, XIE Yan, SHENG Xuejia, et al. Novel collection equipment loaded with superhydrophobic sponge for continuous oil/water separation from offshore environments[J]. Coatings, 2023, 13(3): 573.
5	YANG Fan, HAO Longbin, ZHU Yanan, et al. Preparation of graphene modified melamine sponge and solar-assisted cleanup of heavy oil spills[J]. Journal of Environmental Chemical Engineering, 2022, 10(3): 107779.
6	BAO Zhijie, BING Naici, YAO Hurong, et al. Three-dimensional interpenetrating network phase-change composites with high photothermal conversion and rapid heat storage and release[J]. ACS Applied Energy Materials, 2021, 4(8): 7710-7720.
7	PLUTNAR Jan, PUMERA Martin, SOFER Zdeněk. The chemistry of CVD graphene[J]. Journal of Materials Chemistry C, 2018, 6(23): 6082-6101.
8	PAUL Joyel, AHANKARI Sandeep S. Nanocellulose-based aerogels for water purification: A review[J]. Carbohydrate Polymers, 2023, 309: 120677.
9	Ton That BUU, Vo Hoai SON, Nguyen Thanh Hoai NAM, et al. Three-dimensional ZnO-TiO₂/graphene aerogel for water remediation: The screening studies of adsorption and photodegradation[J]. Ceramics International, 2023, 49(6): 9868-9882.
10	ZHU Wei, JIANG Xueliang, LIU Fangjun, et al. Preparation of chitosan-graphene oxide composite aerogel by hydrothermal method and its adsorption property of methyl orange[J]. Polymers, 2020, 12(9): 2169.
11	刁帅, 刘会娥, 陈爽, 等. 软模板法石墨烯气凝胶的可控制备及其吸油性能[J]. 化工进展, 2020, 39(7): 2742-2750.
	DIAO Shuai, LIU Hui’e, CHEN Shuang, et al. Controllable preparation of graphene aerogels with soft templates and its adsorption on oils[J]. Chemical Industry and Engineering Progress, 2020, 39(7): 2742-2750.
12	JIANG Leilei, HU Xuebing, YANG Boshen, et al. Preparation of porous diethylene triamine reduced graphene oxide aerogel for efficient pollutant dye adsorption[J]. Journal of Porous Materials, 2023, 30(5): 1485-1497.
13	ZHANG Peng, CHEN Yizhi, WENG Hanqin, et al. Reduced graphene oxide composite aerogel prepared by europium-assisting radiation reduction as a broad-spectrum adsorbent for organic pollutants[J]. Journal of Materials Chemistry A, 2023, 11(6): 2804-2813.
14	CUI Yan, KANG Weiwei, HU Jifan. Effectiveness and mechanisms of the adsorption of phenol from wastewater onto N-doped graphene oxide aerogel[J]. Journal of Water Process Engineering, 2023, 53: 103665.
15	GUPTA Shobhnath P, WALKE Pravin S. Scalable multifunctional ultralight mesoporous micro yarn carbon for excellent durable supercapacitor and tremendous oils sorbent[J]. Chemical Engineering Journal, 2023, 456: 141011.
16	CAO Ning, Qian LYU, LI Jin, et al. Facile synthesis of fluorinated polydopamine/chitosan/reduced graphene oxide composite aerogel for efficient oil/water separation[J]. Chemical Engineering Journal, 2017, 326: 17-28.
17	CONG Longliang, LI Xiaoru, MA Lichun, et al. High-performance graphene oxide/carbon nanotubes aerogel-polystyrene composites: Preparation and mechanical properties[J]. Materials Letters, 2018, 214: 190-193.
18	AFROZE Jannatul Dil, TONG Liyong, ABDEN Md Jaynul, et al. Hierarchical honeycomb graphene aerogels reinforced by carbon nanotubes with multifunctional mechanical and electrical properties[J]. Carbon, 2021, 175: 312-321.
19	KABIRI Shervin, TRAN Diana N H, ALTALHI Tariq, et al. Outstanding adsorption performance of graphene-carbon nanotube aerogels for continuous oil removal[J]. Carbon, 2014, 80: 523-533.
20	LIU Hui’e, TIAN Xiaowen, XIANG Xiaoxiao, et al. Preparation of carboxymethyl cellulose/graphene composite aerogel beads and their adsorption for methylene blue[J]. International Journal of Biological Macromolecules, 2022, 202: 632-643.
21	HU Yuwei, JIANG Yijing, NI Lingyu, et al. An elastic MOF/graphene aerogel with high photothermal efficiency for rapid removal of crude oil[J]. Journal of Hazardous Materials, 2023, 443: 130339.
22	SUN Anqi, HOU Xuan, HU Xiangang. Super-performance photothermal conversion of 3D macrostructure graphene-CuFeSe₂ aerogel contributes to durable and fast clean-up of highly viscous crude oil in seawater[J]. Nano Energy, 2020, 70: 104511.
23	WANG Chengjun, WANG Linqiang, LIANG Weidong, et al. Enhanced light-to-thermal conversion performance of all-carbon aerogels based form-stable phase change material composites[J]. Journal of Colloid and Interface Science, 2022, 605: 60-70.
24	LUO Zhuo, WANG Xiaotong, YANG Dongzhi, et al. Photothermal hierarchical carbon nanotube/reduced graphene oxide microspherical aerogels with radially orientated microchannels for efficient cleanup of crude oil spills[J]. Journal of Colloid and Interface Science, 2020, 570: 61-71.
25	YANG Feng, WANG Meng, ZHANG Daqi, et al. Chirality pure carbon nanotubes: Growth, sorting, and characterization[J]. Chemical Reviews, 2020, 120(5): 2693-2758.
26	GUO Jing, PENG Ruixuan, ZHANG Xiaolong, et al. Perforated carbon nanotube film assisted growth of uniform monolayer MoS₂ [J]. Small, 2023, 19(23): e2300766.
27	NOVIKOV Ilya V, KHABUSHEV Eldar M, KRASNIKOV Dmitry V, et al. Residence time effect on single-walled carbon nanotube synthesis in an aerosol CVD reactor[J]. Chemical Engineering Journal, 2021, 420: 129869.
28	HUMMERS William S, OFFEMAN Richard E. Preparation of graphitic oxide[J]. Journal of the American Chemical Society, 1958, 80(6): 1339.
29	王振有, 刘会娥, 朱佳梦, 等. 乳液法制备聚乙烯醇-石墨烯气凝胶及其对纯有机物的吸附[J]. 化工学报, 2019, 70(3): 1152-1162.
	WANG Zhenyou, LIU Hui’e, ZHU Jiameng, et al. Preparation of polyvinyl alcohol-graphene aerogel by emulsion method and its adsorption on pure organics[J]. CIESC Journal, 2019, 70(3): 1152-1162.
30	COTE Laura J, KIM Franklin, HUANG Jiaxing. Langmuir-Blodgett assembly of graphite oxide single layers[J]. Journal of the American Chemical Society, 2009, 131(3): 1043-1049.
31	GUO Qilin, CHEN Shuang, LIU Zexin, et al. Preparation and performance evaluation of graphene/hydroxypropyl methylcellulose composite aerogel for high viscosity oil adsorption[J]. Journal of Environmental Chemical Engineering, 2022, 10(5): 108312.
32	ZHU Shuyi, XU Shuai, GUO Yujing, et al. Defect damping-enhanced plasmonic photothermal conversion[J]. ACS Nano, 2023, 17(11): 10300-10312.
33	QI Yuhang, SONG Lizhu, OUYANG Shuxin, et al. Photoinduced defect engineering: Enhanced photothermal catalytic performance of 2D black In₂O_3- _x nanosheets with bifunctional oxygen vacancies[J]. Advanced Materials, 2020, 32(6): e1903915.

材料	油水比	m₀/g	V_A/cm³	ρ_A×10³/g·cm^-3	V_pore/cm³·g^-1
STRGA	0.8∶1	0.0115	2.16	5.32	188
CNTs/STRGA-1/3-0.4-3	0.4∶1	0.0163	2.12	7.68	130
CNTs/STRGA-1/3-0.6-3	0.6∶1	0.0146	2.14	6.83	146
CNTs/STRGA-1/3-0.8-3	0.8∶1	0.0130	2.16	6.02	166
CNTs/STRGA-1/3-0.85-3	0.85∶1	材料无法成形
CNTs/STRGA-1/3-0.9-3	0.9∶1	材料无法成形

材料	油水比	m₀/g	V_A/cm³	ρ_A×10³/g·cm^-3	V_pore/cm³·g^-1
STRGA	0.8∶1	0.0115	2.16	5.32	188
CNTs/STRGA-1/3-0.4-3	0.4∶1	0.0163	2.12	7.68	130
CNTs/STRGA-1/3-0.6-3	0.6∶1	0.0146	2.14	6.83	146
CNTs/STRGA-1/3-0.8-3	0.8∶1	0.0130	2.16	6.02	166
CNTs/STRGA-1/3-0.85-3	0.85∶1	材料无法成形
CNTs/STRGA-1/3-0.9-3	0.9∶1	材料无法成形

材料	1次压缩的最大应力/kPa	300次压缩的最大应力/kPa	应力损失/%
CNTs/STRGA-1/3-0.8-1	4.11	3.06	25.55
CNTs/STRGA-1/3-0.8-2	7.12	5.98	16.01
CNTs/STRGA-1/3-0.8-3	8.33	7.00	15.96
CNTs/STRGA-1/3-0.8-4	8.38	7.06	15.75

材料	1次压缩的最大应力/kPa	300次压缩的最大应力/kPa	应力损失/%
CNTs/STRGA-1/3-0.8-1	4.11	3.06	25.55
CNTs/STRGA-1/3-0.8-2	7.12	5.98	16.01
CNTs/STRGA-1/3-0.8-3	8.33	7.00	15.96
CNTs/STRGA-1/3-0.8-4	8.38	7.06	15.75

材料	m₀/g	(m_max-m₀)/g	V_oil/cm³·g^-1	C_max/g·g^-1	v/g·g^-1·min^-1	η/%
STRGAs	0.0115	1.7255	157.61	150.04	3.66	84.05
CNTs/STRGA-1/3-0.4-3	0.0163	1.6339	105.29	100.24	3.85	81.15
CNTs/STRGA-1/3-0.6-3	0.0146	1.6791	120.81	115.01	5.00	82.77
CNTs/STRGA-1/3-0.8-3	0.0130	1.6986	137.24	130.66	6.88	82.83