中空碳纳米球与UiO-66复合材料的制备及其VOCs吸附性能

doi:10.15541/jim20250445

无机材料学报 ›› 2026, Vol. 41 ›› Issue (9): 1285-1293.DOI: 10.15541/jim20250445

中空碳纳米球与UiO-66复合材料的制备及其VOCs吸附性能

王涵¹(), 清江², 黄红花³, 王红宁¹(), 姚超¹, 陈若愚¹

¹ 常州大学江苏省精细石化工程重点实验室, 常州 213164
² 上海海关工业产品与原材料检验检测技术中心, 上海 200135
³ 青岛海关技术中心, 青岛 266002

收稿日期:2025-11-03 修回日期:2026-01-17 出版日期:2026-09-20 网络出版日期:2026-02-05
通讯作者: 王红宁, 副教授. E-mail: hnwang@cczu.edu.cn
作者简介:王涵(2000-), 女, 硕士研究生. E-mail: wh15651297162@163.com
基金资助:
青岛海关技术中心(266002);国家重点研发计划(2023YFC3306301)

Hollow Carbon Nanospheres/UiO-66 Composites: Fabrication and VOCs Adsorption Performance

WANG Han¹(), QING Jiang², HUANG Honghua³, WANG Hongning¹(), YAO Chao¹, CHEN Ruoyu¹

¹ Jiangsu Province Key Laboratory of Fine Petrochemical Engineering, Changzhou University, Changzhou 213164, China
² Technical Center for Industrial Product and Raw Material Inspection and Testing, Shanghai Customs, Shanghai 200135, China
³ Technology Center of Qingdao Customs, Qingdao 266002, China

Received:2025-11-03 Revised:2026-01-17 Published:2026-09-20 Online:2026-02-05
Contact: WANG Hongning, associate professor. E-mail:hnwang@cczu.edu.cn
About author:WANG Han (2000-), female, Master candidate. E-mail: wh15651297162@163.com
Supported by:
Technology Center of Qingdao Customs(266002);National Key Research and Development Program of China(2023YFC3306301)

摘要/Abstract

摘要：

挥发性有机化合物(VOCs)对环境可持续性与公共健康构成显著威胁。然而, 现有吸附剂常难以兼顾高容量与稳定性。本研究以正硅酸四丙酯为硅源, 在碱性条件下合成中空碳纳米球(HCNS), 并通过改变碱溶液浓度、活化温度来调节HCNS的表面羟基含量, 得到一系列HCNS-x; 再将HCNS-x与比表面积大、热稳定性良好的UiO-66进行复合, 制得HCNS-x/UiO-66复合材料。通过各种表征测试研究其表面性质和结构, 结果表明, 在3 mol/L NaOH、60 ℃的活化条件下, HCNS-2的表面羟基含量最高, 并且, HCNS-2/UiO-66复合材料具有最佳的孔结构参数(比表面积为3694 m²·g^-1, 孔体积为2.53 cm³·g^-1, 平均孔径为6.9 nm)。HCNS-2/UiO-66的静态甲苯吸附容量为2.305 g·g^-1, 是UiO-66 (0.220 g·g^-1)的10.5倍, HCNS (1.436 g·g^-1)的1.6倍; 动态甲苯吸附结果表明HCNS-2/UiO-66具有最优异的甲苯吸附性能, 平衡吸附容量为2.140 g·g^-1, 这与其较大的比表面积和优化的孔结构有关。此外, 循环实验表明, HCNS-2/UiO-66在多次动态吸附-脱附循环后仍保持性能稳定, 其饱和吸附容量始终维持在约2.15 g·g^-1。本研究通过对HCNS进行表面改性, 优化其与UiO-66的界面结合, 从而构建了兼具高吸附容量和稳定性的VOCs吸附材料。

关键词: 中空碳纳米球, 复合材料, 挥发性有机化合物, 吸附, 表面改性

Abstract:

Volatile organic compounds (VOCs) significantly threaten both environmental sustainability and public health. However, it remains challenging to combine high capacity and stability in most existing adsorbents. In this work, hollow carbon nanospheres (HCNS) were synthesized under alkaline conditions using tetrapropyl orthosilicate as the silicon source, followed by modulation of their surface hydroxyl content through variations in alkali concentration or temperature to yield a series of HCNS-x. These HCNS-x were then composited with UiO-66, which possesses a high specific surface area and excellent thermal stability, to prepare HCNS-x/UiO-66 composites. Their surface properties and structures were investigated through various characterization techniques. The results indicated that HCNS-2, activated with 3 mol/L NaOH at 60 ℃, exhibited the highest surface hydroxyl content. Furthermore, its corresponding composite, HCNS-2/UiO-66, demonstrated the most optimal pore structure parameters (a specific surface area as high as 3694 m²·g^-1, a total pore volume of 2.53 cm³·g^-1, and an average pore size of 6.9 nm). Static toluene adsorption tests revealed that the toluene adsorption capacity of HCNS-2/UiO-66 was 2.305 g·g^-1, which was 10.5 times that of pure UiO-66 (0.220 g·g^-1) and 1.6 times that of pristine HCNS (1.436 g·g^-1). Dynamic toluene adsorption breakthrough curve analysis confirmed that HCNS-2/UiO-66 possessed the most excellent toluene adsorption performance with an equilibrium adsorption capacity of 2.140 g·g^-1, which was attributed to its large specific surface area and optimized pore structure. Additionally, cycling tests demonstrated that HCNS-2/UiO-66 maintained stable performance over multiple dynamic adsorption-desorption cycles, demonstrating that its saturated adsorption capacity consistently remained around 2.15 g·g^-1. This study constructed a VOCs adsorbent with high adsorption capacity and stability by modifying the HCNS surface to optimize its interfacial integration with UiO-66.

Key words: hollow carbon nanosphere, composite, volatile organic compound, adsorption, surface modification

中图分类号:

X511

王涵, 清江, 黄红花, 王红宁, 姚超, 陈若愚. 中空碳纳米球与UiO-66复合材料的制备及其VOCs吸附性能[J]. 无机材料学报, 2026, 41(9): 1285-1293.

WANG Han, QING Jiang, HUANG Honghua, WANG Hongning, YAO Chao, CHEN Ruoyu. Hollow Carbon Nanospheres/UiO-66 Composites: Fabrication and VOCs Adsorption Performance[J]. Journal of Inorganic Materials, 2026, 41(9): 1285-1293.

图/表 21

图1 样品的XRD图谱

Fig. 1 XRD patterns of the samples (a) HCNS and HCNS-x samples; (b) UiO-66 and HCNS-x/UiO-66 samples

图2 样品的FT-IR光谱

Fig. 2 FT-IR spectra of the samples (a) HCNS and HCNS-x samples; (b) UiO-66 and HCNS-x/UiO-66 samples

图3 不同活化条件下样品的静态水吸附容量

Fig. 3 Static water adsorption capacities of samples under different activation conditions

图4 样品的SEM照片

Fig. 4 SEM images of the samples (a) UIO-66; (b) HCNS; (c) HCNS-1; (d) HCNS-1/UiO-66; (e) HCNS-2; (f) HCNS-2/UiO-66; (g) HCNS-3; (h) HCNS-3/UiO-66

图5 样品的TEM照片

Fig. 5 TEM images of the samples (a) HCNS; (b) UiO-66; (c) HCNS-1; (d) HCNS-1/UiO-66; (e) HCNS-2; (f) HCNS-2/UiO-66; (g) HCNS-3; (h) HCNS-3/UiO-66

图6 样品的N2吸附-脱附等温线(a, b)和孔径分布曲线(c, d)

Fig. 6 N2 adsorption-desorption isotherms (a, b) and pore size distribution curves (c, d) of the samples

图7 样品的静态甲苯吸附容量

Fig. 7 Static toluene adsorption capacities of the samples (a) UiO-66, HCNS and HCNS-x samples; (b) HCNS+UiO-66, HCNS/UiO-66 and HCNS-x/UiO-66 samples

图8 不同样品的动态甲苯吸附穿透(拟合)曲线

Fig. 8 Dynamic toluene adsorption breakthrough (fitting) curves of different samples

图9 不同温度下HCNS-2/UiO-66的动态甲苯吸附穿透曲线

Fig. 9 Dynamic toluene adsorption breakthrough curves of HCNS-2/UiO-66 at different temperatures

图S1 静态水吸附容量和表面羟基含量的线性关系

Fig. S1 Linear relationship between static water adsorption capacity and density of surface hydroxyl

图S2 不同活化条件下样品的静态水解吸效率

Fig. S2 Static water desorption efficiency of samples under different activation conditions

图S3 HCNS/UiO-66的SEM照片(a)和TEM照片(b)

Fig. S3 SEM image (a) and TEM image (b) of HCNS/UiO-66

图S4 样品的TGA曲线

Fig. S4 TGA curves of the samples

图S5 样品的静态吸附容量(a)和解吸效率(b)

Fig. S5 Static adsorption capacities (a) and desorption efficiencies (b) of the samples

图S6 样品的静态甲苯解吸效率

Fig. S6 Static toluene desorption efficiencies of the samples

表S1 不同样品的静态水吸附容量、解吸效率和表面羟基含量

Table S1 Static water adsorption capacities, desorption efficiencies and density of surface hydroxy of different samples

Sample	Adsorption capacity/(g·g^-1)	Desorption efficiency/%	D/(×10²⁰, g^-1)
HCNS	0.8850	99.62	2.85
HCNS-1	0.9615	99.64	3.03
HCNS-2	1.1020	99.20	3.54
HCNS-3	0.9056	99.44	2.91

表S2 样品的孔结构参数

Table S2 Pore structure parameters of the samples

Sample	S_BET/ (m²·g^-1)	Pore volume, V_t/(cm³·g^-1)	Micropore volume, V_m/(cm³·g^-1)	Pore diameter/nm
HCNS	968	1.25	0.10	5.2
HCNS-1	1069	1.60	0.12	6.0
HCNS-2	1514	2.23	0.62	6.0
HCNS-3	1055	1.13	0.18	5.9
UiO-66	236	0.16	0.10	2.7
HCNS-1/UiO-66	1504	2.47	0.19	6.6
HCNS-2/UiO-66	3694	2.53	0.44	6.9
HCNS-2/UiO-66	1470	2.41	0.14	6.6

表S3 不同样品的动态甲苯吸附参数

Table S3 Dynamic toluene adsorption parameters of different samples

Sample	t_b/min	t_e/min	q_e/(g·g^-1)	Desorption efficiency/%
UiO-66	16	68	0.198	99.5
HCNS-1/UiO-66	68	148	1.586	99.6
HCNS-2/UiO-66-1st	90	210	2.140	98.7
HCNS-2/UiO-66-2nd	90	214	2.150	99.3
HCNS-2/UiO-66-3rd	98	206	2.200	99.7
HCNS-2/UiO-66-4th	94	214	2.230	99.6
HCNS-2/UiO-66-5th	90	212	2.130	99.3
HCNS-3/UiO-66	60	128	1.382	98.9

表S4 不同样品的动态甲苯吸附拟合参数

Table S4 Dynamic toluene adsorption fitting parameters of different samples

Sample	τ₀/min	k′/min^-1	R²
UiO-66	30.9	0.337	0.997
HCNS-1/UiO-66	55.3	0.224	0.997
HCNS-2/UiO-66-1st	122	0.087	0.998
HCNS-2/UiO-66-2nd	118	0.087	0.998
HCNS-2/UiO-66-3rd	114	0.087	0.998
HCNS-2/UiO-66-4th	110	0.092	0.995
HCNS-2/UiO-66-5th	112	0.094	0.995
HCNS-3/UiO-66	77.1	0.194	0.997

表S5 不同类别VOCs吸附剂的性能对比

Table S5 Performance comparison of different categories of VOCs adsorbents

Category	Sample	S_BET/(m²·g^-1)	q_e/(g·g^-1)	Ref.
Porous carbon materials	AC	1654	0.48	[40]
Porous carbon materials	HCNS	968	1.436	This work
Zeolites	ZSM-5	418	0.12	[41]
MOFs	MIL-101	2907	0.55	[42]
MOFs	UiO-66	236	0.220	This work
Composite materials	C/Si	431	0.11	[43]
Composite materials	HCNS-2/UiO-66	3694	2.140	This work

表S6 不同温度下样品的动态甲苯吸附拟合参数

Table S6 Dynamic toluene adsorption fitting parameters of the samples at different temperatures

Sample	t_b/min	t_e/min	q_e/(g·g^-1)	Desorption efficiency/%
HCNS-2/UiO-66-25 ℃	90	210	2.140	98.7
HCNS-2/UiO-66-60 ℃	40	120	1.304	99.2
HCNS-2/UiO-66-80 ℃	20	64	0.639	99.4

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中空碳纳米球与UiO-66复合材料的制备及其VOCs吸附性能

Hollow Carbon Nanospheres/UiO-66 Composites: Fabrication and VOCs Adsorption Performance

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