疏水改性分子筛在高湿度环境下对甲苯的吸附性能

刘东; 齐俊文; 徐遵主; 张纪文; 金小贤; 李健生

doi:10.13205/j.hjgc.202302010

疏水改性分子筛在高湿度环境下对甲苯的吸附性能

doi: 10.13205/j.hjgc.202302010

1. 南京理工大学环境与生物工程学院, 南京 210094;
2. 南京大学环境规划设计研究院集团股份公司, 南京 210093

基金项目:

国家自然科学基金青年项目(52000106)

详细信息

作者简介:
刘东(1994-),男,在读硕士,主要研究方向为工业废气污染控制。liud@njuae.cn

通讯作者:
李健生(1969-),男,教授,主要研究方向为环境纳米技术的开发及水污染控制。lijsh@njust.edu.cn

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出版历程
- 收稿日期: 2022-07-04
- 网络出版日期: 2023-05-25
- 刊出日期: 2023-02-01

ADSORPTION PERFORMANCE OF TOLUENE ON HYDROPHOBIC MODIFIED MOLECULAR SIEVES UNDER HIGH HUMIDITY

1. School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing 210094, China;
2. Nanjing University Academy of Environmental Planning & Design Group, Nanjing 210093, China

摘要

摘要: 工程实践中Y分子筛在高湿度环境下吸附性能大幅降低,通过聚二烯丙基二甲基氯化铵(PDDA)预处理后进行mesoSiO₂壳层生长得到Y@mesoSiO₂,将聚二甲基硅氧烷(PDMS)通过化学气相沉积法接枝到Y@mesoSiO₂壳层上,可获得疏水特性优异的Y@mesoSiO₂-S核壳分子筛。采用SEM、TEM、XRD、XPS和比表面积及孔径分析仪对改性前后Y分子筛形貌和结构进行分析,通过静态和动态吸附实验评价其对水和甲苯的吸附性能。结果表明:mesoSiO₂壳相在核相Y分子筛外表面成功生长,并将PDMS成功接枝在Y@mesoSiO₂壳层后,Y@mesoSiO₂-S的BET比表面积相比Y分子筛增加了2%;静态水蒸气吸附量从298 mg/g降至79 mg/g,动态水蒸气吸附量从245 mg/g降至76 mg/g,材料表面与水接触角得到显著提升。在RH80%时,Y@mesoSiO₂-S和Y分子筛对甲苯的饱和吸附量分别为167.2,2.6 mg/g,相比RH20%,分别降低了6.7%和98.3%。与无mesoSiO₂壳层的Y-S相比,Y@mesoSiO₂-S的BET比表面积增加了46%,其在高湿度环境下(80%RH)对甲苯的饱和吸附量增加了51%。说明通过在Y分子筛与有机硅烷之间引入mesoSiO₂壳层,可有效避免有机硅烷直接接枝在Y分子筛表面造成的孔道堵塞问题,同时提升了Y分子筛的疏水性能,改善其在高湿度环境下对甲苯的吸附性能。
- Y分子筛 /
- 疏水改性 /
- 甲苯 /
- 高湿度环境 /
- 吸附性能
Abstract: Engineering practice showed that the adsorption performance of Y molecular sieve was greatly reduced under high humidity environment. In this paper, Y@mesoSiO₂ was obtained by pretreating polydiallyl dimethylammonium chloride (PDDA) along with the growth of mesoSiO₂ shell on Y molecular sieve. Polydimethylsiloxane (PDMS) was further grafted onto mesoSiO₂ shell to prepare Y@mesoSiO₂-S via chemical vapor deposition method. The morphology and structure of the modified Y molecular sieve were analyzed by SEM, TEM, XRD, XPS, surface area and pore size analyzer. Besides, the adsorption of water and toluene was evaluated by static and dynamic adsorption experiments. The results showed that the mesoSiO₂ shell successfully grew on the outer surface of Y molecular sieve and PDMS was successfully grafted onto the Y@mesoSiO₂ shell. Compared with Y molecular sieve, the BET specific surface area (S_BET) of Y@mesoSiO₂-S increased by 2%; meanwhile, the water contact angle was enhanced significantly, causing the static water absorption decreased from 298 mg/g to 79 mg/g, and the dynamic water absorption decreased from 245 mg/g to 76 mg/g. The saturated adsorption capacity of toluene on Y@mesoSiO₂-S and Y molecular sieve were 167.2 mg/g and 2.6 mg/g at an RH of 80%, respectively, which decreased by 6.7% and 98.3% relatively, compared with an RH of 20%. When compared with Y-S without mesoSiO₂ shell, Y@mesoSiO₂-S presented increased S_BET and the saturated adsorption capacity of toluene with 46% and 51% at an RH of 80%, respectively. This indicated that mesoSiO₂ shell was introduced between Y molecular sieve and PDMS, which could avoid clogging of porosity caused by direct grafting PDMS on the surface of Y molecular sieve. Furthermore, this strategy could improve the hydrophobic property of Y molecular sieve, resulting in enhanced adsorption performance on toluene under high humidity.
- Y molecular sieve /
- hydrophobic modification /
- toluene /
- high humidity /
- adsorption property

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参考文献(24)

[1]	YANG C T, MIAO G, PI Y H, et al. Abatement of various types of VOCs by adsorption/catalytic oxidation:a review[J]. Chemical Engineering Journal, 2019, 370:1128-1153.
[2]	GUO X C, LI X Y, GAN G Q, et al. Functionalized activated carbon for competing adsorption of volatile organic compounds and water[J]. ACS Applied Materials & Interfaces, 2021, 13(47):56510-56518.
[3]	JESUS L, JOSE P, LUISA G S, et al. Removal of chlorinated organic volatile compounds by gas phase adsorption with activated carbon[J]. Chemical Engineering Journal, 2012, 211:246-254.
[4]	ZHANG X Y, GAO B, ANNE E C, et al. Adsorption of VOCs onto engineered carbon materials:a review[J]. Journal of Hazardous Materials, 2017, 338:102-123.
[5]	PARMAR G R, RAO N N. Emerging control technologies for volatile organic compounds[J]. Critical Reviews in Environmental Science and Technology, 2008, 39(1):41-78.
[6]	黄心, 刘荣, 李红梅, 等. VOCs处理技术研究进展[J]. 广州化工, 2021, 49(13):30-34.
[7]	徐遵主,陆朝阳, 张纪文,等. 长三角典型城市工业VOCs处理技术应用状况分析[J]. 环境工程, 2020, 38(1):6.
[8]	冯爱虎, 于洋, 余云, 等. 沸石分子筛及其负载型催化剂去除VOCs研究进展[J]. 化学学报, 2018, 76(10):757-773.
[9]	党小庆, 王琪, 曹利, 等. 吸附法净化工业VOCs的研究进展[J]. 环境工程学报, 2021, 15(11):3479-3492.
[10]	LIU S H, PENG Y, CHEN J J, et al. Engineering surface functional groups on mesoporous silica:towards a humidity-resistant hydrophobic adsorbent[J]. Journal of Materials Chemistry, 2018, 6(28):13769-13777.
[11]	MOTEKI T, LOBO R F. A general method for aluminum incorporation into high-silica zeolites prepared in fluoride media[J]. Chemistry of Materials, 2016, 28(2):638-649.
[12]	ZUO X T, CHENG Q, SENLIN M, et al. Removal of sulfonamide antibiotics from water by high-silica ZSM-5[J]. Water Science and Technology, 2019, 80(3):507-516.
[13]	LI R N, XUE T S, BINGRE R, et al. Microporous zeolite@vertically aligned Mg-Al layered double hydroxide core@shell structures with improved hydrophobicity and toluene adsorption capacity under wet conditions[J]. ACS Applied Materials & Interfaces, 2018, 10(41):34834-34839.
[14]	YU Y F, ZHENG L W, Wang J D. Adsorption behavior of toluene on modified 1X molecular sieves[J]. Journal of the Air & Waste Management Association, 2012, 62(10):1227-1232.
[15]	MENG X, JIN L P, YANG C, et al. Adsorption of toluene on silicalite-1/NaY composites:influence of NaY pretreatment on hydrophobic properties[J]. Applied Organometallic Chemistry, 2012, 35(3):e6118.
[16]	LU S C, LIU Q L, HAN R, et al. Core-shell structured Y zeolite/hydrophobic organic polymer with improved toluene adsorption capacity under dry and wet conditions[J]. Chemical Engineering Journal, 2021, 409:128194.
[17]	YIN T, MENG X, JIN L P, et al. Prepared hydrophobic Y zeolite for adsorbing toluene in humid environment[J]. Microporous and Mesoporous Materials, 2020, 305:110327.
[18]	YOON Y H, NELSON J H. Application of Gas Adsorption Kinetics-Ⅱ. A Theoretical Model for Respirator Cartridge Service Life and Its Practical Applications[J]. American Industrial Hygiene Association Journal, 1984, 45(8):517-524.
[19]	REZAKAZEMI M, SHIRAZIAN S. Lignin-chitosan blend for methylene blue removal:adsorption modeling[J]. Journal of Molecular Liquids, 2019, 274:778-791.
[20]	LEE S H, LEE D K, SHIN C H, et al. Synthesis, characterization, and catalytic properties of zeolites IM-5 and NU-88[J]. Journal of Catalysis, 2003, 215(1):151-170.
[21]	LI X G, YUAN J J, DU J Z, et al. Functionalized ordered mesoporous silica by vinyltriethoxysilane for the removal of volatile organic compounds through adsorption/desorption process[J]. Industrial & Engineering Chemistry Research, 2020, 59(8):3511-3520.
[22]	GAI S L, YANG P P, LI C X, et al. Synthesis of magnetic, up-conversion luminescent and mesoporous core-shell-structured nanocomposites as drug carriers[J]. Advanced Functional Materials, 2010, 20(7):1166-1172.
[23]	MATTOGNO G, RIGHINI G, MONTESPERELLI G, et al. XPS analysis of the interface of ceramic thin films for humidity sensors[J]. Applied Surface Science, 1993, 70(Part-1):363-366.
[24]	SONG W, LIU Z, LIU L P, et al. A solvent evaporation route towards fabrication of hierarchically porous ZSM-11 with highly accessible mesopores[J]. RSC Advances, 2015, 5(39):31195-31204.