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UiO-66/氧化石墨烯的制备及对水中四氯化碳的吸附

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史琳, 叶倩玲, 杨琦, 刘兆香. UiO-66/氧化石墨烯的制备及对水中四氯化碳的吸附[J]. 环境工程学报, 2019, 13(5): 1063-1072. doi: 10.12030/j.cjee.201810060
引用本文: 史琳, 叶倩玲, 杨琦, 刘兆香. UiO-66/氧化石墨烯的制备及对水中四氯化碳的吸附[J]. 环境工程学报, 2019, 13(5): 1063-1072. doi: 10.12030/j.cjee.201810060
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SHI Lin, YE Qianling, YANG Qi, LIU Zhaoxiang. Absorption of carbon tetrachloride from aqueous solution by synthesized UiO-66/graphene oxide[J]. Chinese Journal of Environmental Engineering, 2019, 13(5): 1063-1072. doi: 10.12030/j.cjee.201810060
Citation: SHI Lin, YE Qianling, YANG Qi, LIU Zhaoxiang. Absorption of carbon tetrachloride from aqueous solution by synthesized UiO-66/graphene oxide[J]. Chinese Journal of Environmental Engineering, 2019, 13(5): 1063-1072. doi: 10.12030/j.cjee.201810060
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UiO-66/氧化石墨烯的制备及对水中四氯化碳的吸附

  • 1.

    中国地质大学北京，水资源与环境工程北京市重点实验室，北京 100083

  • 2.

    中国地质大学北京，地下水循环与环境演化教育部重点实验室，北京 100083

  • 3.

    环境保护部，环境保护对外合作中心，北京 100035

  • 基金项目:

    北京市产学研项目51900265005

    国家科技重大专项2009ZX07207-008，2009ZX07419-002，2009ZX07207-001，2015ZX07406005-001

    中央高校基本科研业务费专项资金2652013101，2652013086，2652013087

    国家重大科学仪器设备开发专项2012YQ060115北京市产学研项目(51900265005)

    国家科技重大专项(2009ZX07207-008，2009ZX07419-002，2009ZX07207-001，2015ZX07406005-001)

    中央高校基本科研业务费专项资金(2652013101，2652013086，2652013087)

    国家重大科学仪器设备开发专项(2012YQ060115)

Absorption of carbon tetrachloride from aqueous solution by synthesized UiO-66/graphene oxide

  • 1.

    Beijing Key Laboratory of Water Resource & Environmental Engineering, China University of Geoscience Beijing, Beijing 100083, China

  • 2.

    Key Laboratory of Groundwater Circulation and Environmental Evolution, Ministry of Education, China University of Geoscience Beijing, Beijing 100083, China

  • 3.

    Foreign Economic Cooperation Office, Ministry of Environmental Protection, Beijing 100035, China

  • Fund Project:

  • 摘要: 采用溶剂热法制备了UiO-66和UiO-66/氧化石墨烯复合材料；以水中四氯化碳为处理对象，研究了吸附时间、污染物浓度及温度等因素对吸附过程的影响，并对吸附过程进行动力学和热力学模拟探讨。结果表明，当四氯化碳浓度为10 mg·L-1、30 ℃时，吸附反应在6 h达到平衡，四氯化碳的去除率为87.5%。UiO-66/氧化石墨烯材料对四氯化碳的吸附过程符合拟二级动力学模型。热力学结果显示ΔG0、ΔS>0，由此判断吸附过程是自发、吸热和熵增加的过程。UiO-66/氧化石墨烯材料中比表面积、表面分散力和晶体缺陷的增加使其对四氯化碳具有更好的吸附性能。
    Abstract: Nano-sized metal organic framework UiO-66 and UiO-66/graphene oxide composites were prepared using a microwave-assisted solvothermal method. Influences of several parameters, such as time, carbon tetrachloride concentration, and temperature, on the carbon tetrachloride adsorption by UiO-66/graphene oxide composites were investigated. Meanwhile, adsorption kinetics and thermodynamics were also explored. Results showed that the adsorption equilibrium occurred within 6 hours and the removal efficiency of carbon tetrachloride was 87.5% at its initial concentration of 10 mg·L-1 and 30 ℃. A pseudo-second order kinetic model fitted well with the adsorption kinetic process. The negative value of ΔG and positive values of ΔH and ΔS determined through thermodynamics of adsorption indicated that the adsorption was a spontaneous, endothermic and entropy increase process. The adsorption effect of carbon tetrachloride on the UiO-66/GrO was better than UiO-66 owing to the increasing of specific area, dispersion forces and defects on the crystal surface.
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  • [1] BIE P J, FANG X K, LI Z F, et al. Emissions estimates of carbon tetrachloride for 1992-2014 in China[J]. Environmental Pollution, 2017, 224: 670-678.
    [2] ABDELBASSIT M S A, ALHOOSHANI K R, SALEH T A. Silica nanoparticles loaded on activated carbon for simultaneous removal of dichloromethane, trichloromethane, and carbon tetrachloride[J]. Advanced Powder Technology, 2016, 27(4): 1719-1729.
    [3] BHATNAGAR A, HOGLAND W, MARQUES M, et al. An overview of the modification methods of activated carbon for its water treatment applications[J]. Chemical Engineering Journal, 2013, 219: 499-511.
    [4] PASTI L, MARTUCCI A, NASSI M, et al. The role of water in DCE adsorption from aqueous solutions onto hydrophobic zeolites[J]. Microporous and Mesoporous Materials, 2012, 160: 182-193.
    [5] SHEN W Z, GUO Q J, ZHANG Y S, et al. The effect of activated carbon fiber structure and loaded copper, cobalt, silver on the adsorption of dichloroethylene[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2006, 273(1/2/3): 147-153.
    [6] TAMBAT S N, SANE P K, SURESH S, et al. Hydrothermal synthesis of NH2-UiO-66 and its application for adsorptive removal of dye[J]. Advanced Powder Technology, 2018, 29(11): 2626-2632.
    [7] ZHANG S T, CHENG R, WANG J L, et al. Adsorption of diclofenac from aqueous solution using UiO-66-type metal-organic frameworks[J]. Chemical Engineering Journal, 2019, 359: 354-362.
    [8] 余阳, 陈团伟, 甄文博, 等. UiO-66(Zr)对As3+的吸附性能及吸附动力学研究[J]. 食品与机械, 2016, 32(6): 61-67.
    [9] 杨清香, 任爽爽, 赵倩倩, 等. 磁性UiO-66复合材料的合成及其对水体中硝基酚有机分子的吸附性能[J]. 无机化学学报, 2017, 33(5): 843-852.
    [10] GE L, WANG L, RUDOLPH V, et al. Hierarchically structured metal-organic framework/vertically-aligned carbon nanotubes hybrids for CO2 capture[J]. RSC Advances, 2013, 3(47): 25360-25366.
    [11] PRASANTH K P, RALLAPALLI P, RAJ M C, et al. Enhanced hydrogen sorption in single walled carbon nanotube incorporated MIL-101 composite metal-organic framework[J]. International Journal of Hydrogen Energy, 2011, 36(13): 7594-7601.
    [12] ANBIA M, SHEYKHI S. Preparation of multi-walled carbon nanotube incorporated MIL-53-Cu composite metal-organic framework with enhanced methane sorption[J]. Journal of Industrial and Engineering Chemistry, 2013, 19(5): 1583-1586.
    [13] ZHOU Y, ZHOU L, ZHANG X H, et al. Preparation of zeolitic imidazolate framework-8/graphene oxide composites with enhanced VOCs adsorption capacity[J]. Microporous and Mesoporous Materials, 2016, 225: 488-493.
    [14] ZHAO Y X, SEREDYCH M, ZHONG Q, et al. Superior performance of copper based MOF and aminated graphite oxide composites as CO2 adsorbents at room temperature[J]. ACS Applied Materials & Interfaces, 2013, 5(11): 4951-4959.
    [15] ZHANG Z Z,WANG H, CHEN X Q, et al. Chromium-based metal-organic framework/mesoporous carbon composite: Synthesis, characterization and CO2 adsorption[J]. Adsorption, 2015, 21(1/2): 77-86.
    [16] ZHOU X, HUANG W Y, SHI J, et al. A novel MOF/graphene oxide composite GrO@MIL-101 with high adsorption capacity for acetone[J]. Journal of Materials Chemistry A, 2014, 2(13): 4722-4730.
    [17] SUN X J, XIA Q B, ZHAO Z X, et al. Synthesis and adsorption performance of MIL-101(Cr)/graphite oxide composites with high capacities of n-hexane[J]. Chemical Engineering Journal, 2014, 239: 226-232.
    [18] KUMAR R, JAYARAMULU K, MAJI T. K,et al. Hybrid nanocomposites of ZIF-8 with graphene oxide exhibiting tunable morphology, significant CO2 uptake and other novel properties[J]. Chemical Communications, 2013, 49(43): 4947-4949.
    [19] CAO Y, ZHAO Y X, LV Z J, et al. Preparation and enhanced CO2 adsorption capacity of UiO-66/graphene oxide composites[J]. Journal of Industrial and Engineering Chemistry, 2015, 27: 102-107.
    [20] ZHAO Q, YUAN W, LIANG J, et al. Synthesis and hydrogen storage studies of metal-organic framework UiO-66[J]. International Journal of Hydrogen Energy, 2013, 38(29): 13104-13109.
    [21] 韩易潼, 刘民, 李克艳, 等. 高稳定性金属有机骨架UiO-66的合成与应用[J]. 应用化学, 2016, 33(4): 367-378.
    [22] EBRAHIM A M, BANDOSZ T J. Ce(III) doped Zr-based MOFs as excellent NO2 adsorbents at ambient conditions[J]. ACS Applied Materials & Interfaces, 2013, 5(21): 10565-10573.
    [23] JAHAN M, BAO Q, YANG J X, et al. Structure-directing role of graphene in the synthesis of metal-organic framework nanowire[J]. Journal of the American Chemical Society, 2010, 132(41): 14487-14495.
    [24] ZHENG Y, CHE F C, ZHANG B, et al. Ultrahigh adsorption capacities of carbon tetrachloride on MIL-101 and MIL-101/graphene oxide composites[J]. Microporous and Mesoporous Materials, 2018, 263: 71-76.
    [25] 任天昊, 杨智临, 郭琳, 等. UiO-66对废水中二氯苯氧乙酸的吸附特性[J]. 环境科学, 2016, 37(6): 2202-2210.
    [26] PAVAGADHI S, TANG A, SATHISHKUMAR M, et al. Removal of microcystin-LR and microcystin-RR by graphene oxide: Adsorption and kinetic experiments[J]. Water Research, 2013, 47: 4621-4629.
    [27] SALEH T A, ALHOOSHANI K R, ABDELBASSIT M S A, et al. Evaluation of AC/ZnO composite for absorption of dichloromethane, trichloromethane and carbon tetrachloride: Kinetics and isotherms[J]. Journal of the Taiwan Institute of Chemical Engineers, 2015, 55: 159-169.
    [28] ZHAO G X, LI J X, WANG X K. Kinetic and thermodynamic study of 1-naphthol adsorption from aqueous solution to sulfonated graphene nanosheets[J]. Chemical Engineering Journal, 2011, 173(1): 185-190.
    [29] 刘伟, 杨琦, 李博, 等. 磁性石墨烯吸附水中Cr(Ⅵ)研究[J]. 环境科学, 2015, 36(2): 537-544.
    [30] 何春东, 朱雪强, 刘汉湖, 等. 活性氧化铝吸附水中四氯化碳的实验研究[J]. 环境科技, 2012, 25(4): 14-18.
    [31] 彭敏. 粉末活性炭吸附水中四氯化碳试验研究[J]. 供水技术, 2011, 5(2): 18-20.
    [32] 席宏波, 杨琦, 尚海涛, 等. 三氧化二铝超细粉末对水中三氯乙烯吸附特性研究[J]. 地球与环境, 2008, 36(3): 270-275.
    [33] 于谦, 杨春生, 丁成. 1,2二氯苯在3种基质中的吸附研究[J]. 环境工程学报, 2011, 5(7): 1675-1680.
    [34] LI D, QIN L, WANG K, et al. Growth of zeolite crystals with graphene oxide nanosheets[J]. Chemical Communications, 2012, 48(16): 2249-2251.
    [35] ZHANG X Y, GAN B, CREAMER A. E,et al. Adsorption of VOCs onto engineered carbon materials: A review[J]. Journal of Hazardous Materials, 2017, 338:102-123.
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  • 刊出日期:  2019-06-03

UiO-66/氧化石墨烯的制备及对水中四氯化碳的吸附

  • 1. 中国地质大学北京，水资源与环境工程北京市重点实验室，北京 100083
  • 2. 中国地质大学北京，地下水循环与环境演化教育部重点实验室，北京 100083
  • 3. 环境保护部，环境保护对外合作中心，北京 100035
基金项目:

北京市产学研项目51900265005

国家科技重大专项2009ZX07207-008，2009ZX07419-002，2009ZX07207-001，2015ZX07406005-001

中央高校基本科研业务费专项资金2652013101，2652013086，2652013087

国家重大科学仪器设备开发专项2012YQ060115北京市产学研项目(51900265005)

国家科技重大专项(2009ZX07207-008，2009ZX07419-002，2009ZX07207-001，2015ZX07406005-001)

中央高校基本科研业务费专项资金(2652013101，2652013086，2652013087)

国家重大科学仪器设备开发专项(2012YQ060115)

摘要: 采用溶剂热法制备了UiO-66和UiO-66/氧化石墨烯复合材料；以水中四氯化碳为处理对象，研究了吸附时间、污染物浓度及温度等因素对吸附过程的影响，并对吸附过程进行动力学和热力学模拟探讨。结果表明，当四氯化碳浓度为10 mg·L-1、30 ℃时，吸附反应在6 h达到平衡，四氯化碳的去除率为87.5%。UiO-66/氧化石墨烯材料对四氯化碳的吸附过程符合拟二级动力学模型。热力学结果显示ΔG0、ΔS>0，由此判断吸附过程是自发、吸热和熵增加的过程。UiO-66/氧化石墨烯材料中比表面积、表面分散力和晶体缺陷的增加使其对四氯化碳具有更好的吸附性能。

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