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硅胶表面TEOS疏水化改性及吸附VOCs特性
Hydrophobic modification of TEOS on silica gel surface and its adsorption characteristics of VOCs
以正硅酸乙酯（TEOS）为疏水改性剂，通过硅胶表面的羟基接枝反应，得到具备一定疏水性的改性硅胶；利用BET、FT-IR、XRD和TG-DTG等手段对改性硅胶的结构及稳定性进行了表征；在此基础上考察了改性硅胶对各类有机废气的吸附性能.结果表明，TEOS成功接枝在了硅胶表面，改性硅胶不仅具备一定的疏水性，而且机械强度增加到原来的66.85%，稳定性也都得到了提高； 550℃空气下焙烧后的改性硅胶仍具有疏水性且吸附容量是焙烧之前的2倍；在高湿度高浓度的废气治理中，TEOS改性硅胶表现出更高的吸附能力和优良的热再生性能.高浓度下改性硅胶的吸附容量是低浓度下的10倍且不受水汽的影响；改性硅胶循环10次的吸附/脱附几乎不变，且在一定条件下，15~30min就达到90%的脱附率.
Volatile organic compounds (VOCs) have become one of the main atmospheric pollutants. Most of VOCs contain a large amount of water vapor, and the relative humidity (RH) is >60%. Therefore, it is crucial to developing hydrophobic adsorbents. In this contribution, tetraethyl orthosilicate (TEOS) was used as a hydrophobic agent to modify the surface of hydrophilic silica gel and prepare the hydrophobic silica gel through hydroxyl grafting reaction. The structure and stability of the adsorbent after grafting reaction was characterized by BET, FT-IR, XRD and TG-DTG. The performances of adsorption on various VOCs were investigated. The results shown that TEOS was successfully grafted on the surface of silica gel and hydrophobic silica gel was prepared. In addition, the mechanical strength has been increased to 66.85%, and stability of silica gel have been improved, the adsorbent after calcination in air at 550℃ is still hydrophobic and its adsorption capacity is twice than before. Last but the most important, higher adsorption capacity of VOCs as well as excellent thermal regeneration of this hydrophobic silica gel could be received under the conditions of high humidity and high concentration VOCs. The adsorption capacity of the hydrophobic silica gel at high concentration was 10 times than that at the low concentration and not affected by water vapor; the adsorption/desorption of the silica gel for 10 cycles was almost unchanged and the desorption rate of 90% was reached in 15-30min under certain conditions.
adsorption / hydrophobic / regeneration / silica / VOCs
[1] Zhao Q, Li Y J, Chai X L, et al. Interaction of inhalable volatile organic compounds and pulmonary surfactant:Potential hazards of VOCs exposure to lung[J]. Journal of Hazardous Materials, 2019,369:512-520.
[2] 李勤勤,张志娟,李杨,等.石油炼化无组织VOCs的排放特征及臭氧生成潜力分析[J]. 中国环境科学, 2016,36(5):1323-1331. Li Q Q, Zhang Z J, Li Y, et al. Characteristics and ozone formation potential of fugitive volatile organic compounds(VOCs) emitted from petrochemical industry in Pearl River Delta[J]. China Environmental Science, 2016,36(5):1323-1331.
[3] 何梦林,肖海麟,陈小方,等.化工园区基于排放环节的VOCs排放特征研究[J]. 中国环境科学, 2017,37(1):38-48. He M L, Xiao H L, Chen X F, et al. Emission characteristics of volatile organic compounds in chemical industry park based on emission links[J]. China Environmental Science, 2017,37(1):38-48.
[4] Zhu Q Y, Tang X, Feng S S, et al. ZIF-8@SiO2 composite nanofiber membrane with bioinspired spider web-like structure for efficient air pollution control[J]. Journal of Membrane Science, 2019,581:252-261.
[5] 姚森,魏巍,程水源,等.轻型汽油车VOCs排放特征及其大气反应活性[J]. 中国环境科学, 2016,36(10):2923-2929. Yao S, Wei W, Cheng S Y, et al. Emission characteristics and chemical reactivity of volatile organic compounds from light-duty gasoline vehicles[J]. China Environmental Science, 2016,36(10):2923-2929.
[6] Tham K W, Wargocki P, Tan Y F. Indoor environmental quality, occupant perception, prevalence of sick building syndrome symptoms, and sick leave in a Green Mark Platinum-rated versus a non-Green Mark-rated building:A case study[J]. Science and Technology for the Built Environment, 2015,21(1):35-44.
[7] Kamal M S, Razzak S A, Hossain M M. Catalytic oxidation of volatile organic compounds (VOCs)-A review[J]. Atmospheric Environment, 2016,140:117-134.
[8] Kim K J, Kang C S, You Y J, et al. Adsorption-desorption characteristics of VOCs over impregnated activated carbons[J]. Catalysis Today, 2005,111(3):223-228.
[9] Yang P, Fan S K, Chen Z Y, et al. Synthesis of Nb2O5 based solid superacid materials for catalytic combustion of chlorinated VOCs[J]. Applied Catalysis B-Environmental, 2018,239:114-124.
[10] Bai G M, Dai H X, Deng J G, et al. The microemulsion preparation and high catalytic performance of mesoporous NiO nanorods and nanocubes for toluene combustion[J]. Chemical Engineering Journal, 2013,219:200-208.
[11] Zou W X, Gao B, et al. Integrated adsorption and photocatalytic degradation of volatile organic compounds (VOCs) using carbon-based nanocomposites:A critical review[J]. Chemosphere, 2019,218:845-859.
[12] Sheng Y, Zhang L, Wang Y Q, et al. Explore energy saving operation strategy:Indoor VOCs removal performance of silica gel rotor in clean-air heat pump system at low regeneration air temperature[J]. Energy & Buildings, 2019:202.
[13] Rioland G, Nouali H, Daou T J, et al. Adsorption of volatile organic compounds in composite zeolites pellets for space decontamination[J]. Adsorption-Journal of the International Adsorption Society, 2017, 23(2/3):395-403.
[14] Parmar G R, Rao N N. Emerging control technologies for volatile organic compounds[J]. Critical Reviews in Environmental Science and Technology, 2009,39(1):41-78.
[15] Zhou K, Ma W W, Zeng Z, et al. Experimental and DFT study on the adsorption of VOCs on activated carbon/metal oxides composites[J]. Chemical Engineering Journal, 2019,372:1122-1133.
[16] Zhou B, Sun B, Qiu W J, et al. Adsorption/desorption of toluene on a hypercrosslinked polymeric resin in a highly humid gas stream[J]. Chinese Journal of Chemical Engineering, 2019,27(4):863-868.
[17] Park E J, Seo H O, Kim Y D. Influence of humidity on the removal of volatile organic compounds using solid surfaces[J]. Catalysis Today, 2017,295:3-13.
[18] Areerob T, Grisdanurak N, Chiarakorn S. Utilization of rice husk silica as adsorbent for BTEX passive air sampler under high humidity condition[J]. Environmental Science and Pollution Research, 2016, 23(6):5538-5548.
[19] Liu H B, Yang B, Xue N D. Enhanced adsorption of benzene vapor on granular activated carbon under humid conditions due to shifts in hydrophobicity and total micropore volume[J]. Journal of Hazardous Materials, 2016,318:425-432.
[20] Zhu M P, Tong Z F, Zhao Z X, et al. A Microporous graphitized biocarbon with high adsorption capacity toward benzene volatile organic compounds (VOCs) from humid air at ultralow pressures[J]. Industrial & Engineering Chemistry Research, 2016,55(13):3765-3774.
[21] Sahar T, Aneeqa S, A C U, et al. Transparent hydrophobic hybrid silica films by green and chemical surfactants[J]. ACS omega, 2019,4(8):13543-13552.
[22] Lu H F, Cao J J, Zhou Y, et al. Novel hydrophobic PDVB/R-SiO2 for adsorption of volatile organic compounds from highly humid gas stream[J]. Journal of Hazardous Materials, 2013,262:83-90.
[23] Lu X A, He J Q, Xie J, et al. Preparation of hydrophobic hierarchical pore carbon-silica composite and its adsorption performance toward volatile organic compounds[J]. Journal of Environmental Sciences, 2019:39-48.
[24] Angulo-Olais R, Illescas J F, Pliego A, et al. Gel Point Determination of TEOS-Based Polymeric Materials with Application on Conservation of Cultural Heritage Buildings[J]. Advances in Condensed Matter Physics, 2018.
[25] Ferri L D, Lorenzi A, Lottici P P. OctTES/TEOS system for hybrid coatings:real-time monitoring of the hydrolysis and condensation by Raman spectroscopy[J]. Journal of Raman Spectroscopy, 2016,47(6):699-705.
[26] 睢文杰,赵文杰,张星,等.铜合金表面巯基官能有机硅溶胶-凝胶涂层中TEOS含量对其防腐性能的影响[J]. 中国腐蚀与防护学报, 2016,36(1):52-58. Zhan W J, Zhao W J, Zhang X, et al. Influence of TEOS content on anti-corrosion property of mercapto functional organic silane based sol-gel coating on copper alloy surface[J]. Journal of Chinese Society for Corrosion and Protection, 2016,36(1):52-58.
[27] Ferri L D, Lottici P P, Lorenzi A, et al. Study of silica nanoparticles-polysiloxane hydrophobic treatments for stone-based monument protection[J]. Journal of Cultural Heritage, 2011,12(4):356-363.
[28] Lampakis D, Manoudis P N, Karapanagiotis I. Monitoring the polymerization process of Si-based superhydrophobic coatings using Raman spectroscopy[J]. Progress in Organic Coatings, 2013,76(2/3):488-494.
[29] Ferri L D, Lottici P P, Lorenzi A, et al. Hybrid sol-gel based coatings for the protection of historical window glass[J]. Journal of Sol-Gel Science and Technology, 2013,66(2):253-263.
[30] Wang Y N, Dai X Y, Xu T L, et al. Preparation and anticorrosion properties of silane grafted nano-silica/epoxy composite coating[J]. Chemical Journal of Chinese Universities-Chinese, 2018,39(7):1564-1572.
[31] Agustín-Sáenz C, Machado M, Zubillaga O, et al. Hydrophobic and spectrally broadband antireflective methyl-silylated silica coatings with high performance stability for concentrated solar applications[J]. Solar Energy Materials and Solar Cells, 2019:200.
[32] Wang H M, Tang M, Zhang K, et al. Functionalized hollow siliceous spheres for VOCs removal with high efficiency and stability[J]. Journal of Hazardous Materials, 2014,268:115-123.
[33] 刘雅哲,盖鸿玮,肖如亭.微球硅胶负载TS-1的制备、表征及催化苯羟基化的研究[J]. 天津理工大学学报, 2011,27(1):69-72. Liu Y Z, Gai H W, Xiao R T. Preparation, characterization and study on catalytic properties for hydroxylation of benezen of TS-1loaded on microspheric silica gel[J]. Journal of Tianjin University of Technology, 2011,27(1):69-72.
[34] Dolatzadeh F, Jalili M M, Moradian S. Influence of various loadings of hydrophilic or hydrophobic silica nanoparticles on water uptake and porosity of a polyurethane coating[J]. Materials and Corrosion-Werkstoffe Und Korrosion, 2013,64(7):609-618.
[35] Chen C, Zhang N, Li W, et al. Water contact angle dependence with hydroxyl functional groups on silica surfaces under CO2 sequestration conditions[J]. Environmental Science & Technology, 2015,49(24):14680-14687.
[36] Jang S C, Yang S I, Oh S G, et al. Adsorption dynamics and effects of carbon to zeolite ratio of layered beds for multicomponent gas adsorption[J]. Korean Journal of Chemical Engineering, 2011,28(2):583-590.
[37] Zhang D D, Cao J, et al. Dynamic adsorption model fitting studies of typical VOCs using commercial activated carbon in a fixed bed[J]. Water Air and Soil Pollution, 2018,229(6).
国家自然科学基金（21506194，21676255）；浙江省自然科学基金（Y16B070025）；浙江省公益技术项目（2017C03007）；浙江省科技厅重点研发项目（2017C33106）
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