石化行业及生产生活中不可避免的排放挥发性有机物(VOCs),油气是常见的VOCs来源,其主要轻质组分是己烷。吸附法是常见的去除VOCs的方法,成本低效率高。为了提升吸附剂的吸附效率,使用溶剂热法制备了UiO-66和UiO-66-NH2,并使用苯甲酸进行缺陷合成改变其孔结构与比表面积,并对其进行了77K氮气(N2)、273K CO2吸附测试,通过X射线衍射、扫描电子显微镜以及热重分析等手段进行表征分析。在30℃、80℃、120℃这3个典型温度下进行正己烷吸附测试及耐久性测试。结果表明:所制UiO-66的BET比表面积可高达1688.57m2/g,1:20当量苯甲酸改性UiO-66吸附容量高达4.47mmol/g,且具有优秀的稳定性。随着温度变化,不同孔径分布在不同温度环境下的吸附剂性能衰减不同。
Volatile organic compounds (VOCs) are inevitably emitted in the petrochemical industry,production and vapor.Oil vapor is a common source of VOCs and its main light component is hexane.The adsorption method is a common method to remove VOCs with low cost and high efficiency.In order to improve the adsorption efficiency of the adsorbent,UiO-66 and UiO-66-NH2 were prepared by solvothermal method,and benzoic acid was used for defect synthesis to change their pore structure and specific surface area.The samples were characteried by 77K nitrogen(N2),273K carbon dioxide(CO2) adsorption,X-ray diffraction(XRD),scanning electron microscope observation (SEM) and thermogravimetric analysis (TG).The n-hexane adsorption test and durability test were performed at three typical temperatures of 30℃,80℃,and 120℃.The results shown that the BET specific surface area of the prepared UiO-66 can be as high as 1688.57m2/g,the adsorption capacity was as high as 4.47mmol/g and it had excellent stability.As the temperature changes,the performance degradation of adsorbents with different pore size distributions in different temperature environments was varied.
[1] Krajnak K,Mckinney W,Waugh S,et al.Cardiovascular effects following a single inhalation exposure to crude oil vapor[J].The FASEB Journal,2019,33:513.9.
[2] Spencer D.BP statistical review of world energy statistical review of world[J].BP Statistical Review of World Energy,2019,68:1-69.
[3] Huang W,Fang J,Li F,et al.Numerical simulation and applications of equivalent film thickness in oil evaporation loss evaluation of internal floating-roof tank[J].Process Safety and Environmental Protection,2019,129:74-88.
[4] Yang C,Miao G,Pi Y,et al.Abatement of various types of VOCs by adsorption/catalytic oxidation:a review[J].Chemical Engineering Journal,2019,370:1128-1153.
[5] Lee J E,Ok Y S,Tsang D C W,et al.Recent advances in volatile organic compounds abatement by catalysis and catalytic hybrid processes:a critical review[J].Science of the Total Environment,2020,719:137405.
[6] Khan S A,Tahir F,Baloch A A B,et al.Review of micro-nanoscale surface coatings application for sustaining dropwise condensation[J].Coatings,2019,9(2):117.
[7] Rezaei F,Vanraes P,Nikiforov A,et al.Applications of plasma-liquid systems:a review[J].Materials,2019,12(17):2751.
[8] Pui W K,Yusoff R,Aroua M K.A review on activated carbon adsorption for volatile organic compounds (VOCs)[J].Reviews in Chemical Engineering,2019,35(5):649-668.
[9] KP Veerapandian S,De Geyter N,Giraudon J M,et al.The use of zeolites for VOCs abatement by combining non-thermal plasma,adsorption,and/or catalysis:a review[J].Catalysts,2019,9(1):98.
[10] Sriram G,Kigga M,Uthappa U T,et al.Naturally available diatomite and their surface modification for the removal of hazardous dye and metal ions:a review[J].Advances in Colloid and Interface Science,2020:102198.
[11] Mushtaq F,Zahid M,Bhatti I A,et al.Possible applications of coal fly ash in wastewater treatment[J].Journal of Environmental Management,2019,240:27-46.
[12] Vaitsis C,Sourkouni G,Argirusis C.Metal organic frameworks (MOFs) and ultrasound:a review[J].Ultrasonics Sonochemistry,2019,52:106-119.
[13] Li X,Liu Y,Zhang C,et al.Porous Fe2O3 microcubes derived from metal organic frameworks for efficient elimination of organic pollutants and heavy metal ions[J].Chemical Engineering Journal,2018,336:241-252.
[14] Seidi F,Jouyandeh M,Taghizadeh M,et al.Metal-organic framework (MOF)/epoxy coatings:a review[J].Materials,2020,13(12):2881.
[15] Piscopo C G,Polyzoidis A,Schwarzer M,et al.Stability of UiO-66 under acidic treatment:opportunities and limitations for post-synthetic modifications[J].Microporous and Mesoporous Materials,2015,208:30-35.
[16] Kandiah M,Nilsen M H,Usseglio S,et al.Synthesis and stability of tagged UiO-66 Zr-MOFs[J].Chemistry of Materials,2010,22(24):6632-6640.
[17] Duerinck T,Denayer J F M.Unusual chain length dependent adsorption of linear and branched alkanes on UiO-66[J].Adsorption,2014,20(2-3):251-259.
[18] Pinto M L,Dias S,Pires J.Composite MOF foams:the example of UiO-66/polyurethane[J].ACS Applied Materials & Interfaces,2013,5(7):2360-2363.
[19] Morris W,Doonan C J,Yaghi O M.Postsynthetic modification of a metal-organic framework for stabilization of a hemiaminal and ammonia uptake[J].Inorganic Chemistry,2011,50(15):6853-6855.
[20] Molavi H,Eskandari A,Shojaei A,et al.Enhancing CO2/N2 adsorption selectivity via post-synthetic modification of NH2-UiO-66 (Zr)[J].Microporous and Mesoporous Materials,2018,257:193-201.
[21] Schaate A,Roy P,Godt A,et al.Modulated synthesis of Zr-based metal-organic frameworks:from nano to single crystals[J].Chemistry-A European Journal,2011,17(24):6643-6651.
[22] 黄兴,钟瑞琴.UiO-66系列材料的制备及其吸附分离CO2/CO性能研究[J].化工新型材料,2020,48(7):221-224.
[23] Chang Z W,Lee Y J,Lee D J.Adsorption of hydrogen arsenate and dihydrogen arsenate ions from neutral water by UiO-66-NH2[J].Journal of Environmental Management,2019,247:263-268.
基金资助
国家自然科学基金(51574044);江苏省重点研发计划(产业前瞻与共性关键技术)重点项目(BE2018065)
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