贻贝仿生三维石墨烯制备及对亚甲基蓝的吸附
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摘要
受海洋生物贻贝的启发,利用多巴胺(DA)自聚合作用将氧化石墨烯自组装成三维(3D)石墨烯材料,并对亚甲基蓝(MB)的吸附行为进行研究.结果显示,3D石墨烯材料具有多孔网络结构,孔径约为0.5μm到几十μm,对MB具有良好的吸附性能,最大吸附量为752 mg·g-1,对MB分子是单分子层吸附,吸附行为符合Langmuir等温吸附和准二级反应动力学方程.通过颗粒内扩散模型对其吸附的扩散机理进行研究,发现吸附初期为外表面扩散吸附,后期为孔道缓慢扩散过程.3D石墨烯对MB吸附具有较好的可再生能力,经过5次的吸附-脱附实验,对MB的去除效率降低20.9%.通过考察其对实际水样中MB的吸附效果,3D石墨烯材料表现出较好的实际应用能力,去除效率均在89%以上.
Inspired by marine mussel,three-dimensional( 3D) graphene materials were prepared through the self-assembly of graphene oxide in the presence of dopamine( DA),and the adsorption experiments were performed to investigate the adsorption behavior of the 3D grapheme materials for methylene blue( MB). The results suggested that the 3D graphene materials exhibited a porous network structure with the pore size ranging from 0. 5 to tens of micrometers, and displayed adsorption capacity as high as 752 mg·g~(-1) for MB. The adsorption behavior followed Langmuir adsorption isotherm and pseudo-second-order kinetic model,indicating that the adsorption process was mainly a monolayer process. The intraparticle diffusion model was also used to investigate the diffusion mechanism of the adsorption behavior. The initial adsorption stage resulted from the external surface diffusion,and the later stage represented a gradual intraparticle diffusion. The 3D graphene materials offered excellent reproducible ability,as the removal efficiency decreased only by about 20.9% after 5 cycles of adsorption-desorption experiments. The 3D graphene materials also exhibitedgood practical application ability with MB removal efficiency of 89% in real samples.
Inspired by marine mussel,three-dimensional( 3D) graphene materials were prepared through the self-assembly of graphene oxide in the presence of dopamine( DA),and the adsorption experiments were performed to investigate the adsorption behavior of the 3D grapheme materials for methylene blue( MB). The results suggested that the 3D graphene materials exhibited a porous network structure with the pore size ranging from 0. 5 to tens of micrometers, and displayed adsorption capacity as high as 752 mg·g~(-1) for MB. The adsorption behavior followed Langmuir adsorption isotherm and pseudo-second-order kinetic model,indicating that the adsorption process was mainly a monolayer process. The intraparticle diffusion model was also used to investigate the diffusion mechanism of the adsorption behavior. The initial adsorption stage resulted from the external surface diffusion,and the later stage represented a gradual intraparticle diffusion. The 3D graphene materials offered excellent reproducible ability,as the removal efficiency decreased only by about 20.9% after 5 cycles of adsorption-desorption experiments. The 3D graphene materials also exhibitedgood practical application ability with MB removal efficiency of 89% in real samples.
引文
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[19] JIN L N,ZHAO X S,QIAN X Y,et al. Nickel nanoparticles encapsulated in porous carbon and carbon nanotube hybrids from bimetallic metal-organic-frameworks for highly efficient adsorption of dyes[J]. Journal of Colloid and Interface Science,2018,509:245-253.
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[21] WANG W,JIAO T F,ZHANG Q R,et al. Hydrothermal synthesis of hierarchical core-shell manganese oxide nanocomposites as efficient dye adsorbents for wastewater treatment[J]. RSC Advances,2015,5(69):56279-56285.
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[25]吴艳,罗汉金,王侯,等.改性石墨烯对水中亚甲基蓝的吸附性能研究[J].环境科学,2013,34(11):4333-4340.WU Y,LUO H J,WANG H,et al. Adsorption properties of modified graphene for methylene blue removal fromwastewater[J].Environmental Science,2013,34(11):4333-4340(in Chinese).
[26]徐恩兵,李坤权,朱志强,等.双孔介孔碳的合成及其对亚甲基蓝的吸附[J].环境化学,2015,34(1):137-143.XU E B,LI K Q,ZHU Z Q,et al. Synthesis of mesoporous carbon with dual-pore structure and their adsorption of methylene blue[J].Environmental Chemistry,2015,34(1):137-143(in Chinese).
[27] YANG M L,LIU X L,QI Y C,et al. Preparation ofκ-carrageenan/graphene oxide gel beads and their efficient adsorption for methylene blue[J]. Journal of Colloid And Interface Science,2017,506:669-677.
[28] GUI C X,WANG Q Q,HAO S M,et al. Sandwichlike magnesium silicate/reduced graphene oxide nanocomposite for enhanced Pb2+and methylene blue adsorption[J]. ACS Applied Materials&Interfaces,2014,6(16):14653-14659.
[29] LIU C Y,LIU H Y,XU A R,et al. In situ reduced and assembled three-dimensional graphene aerogel for efficient dye removal[J].Journal of Alloys and Compounds,2017,714:522-529.
[30] THEYDAN S K,AHMED M J. Adsorption of methylene blue onto biomass-based activated carbon by Fe Cl3activation:Equilibrium,kinetics,and thermodynamic studies[J]. Journal of Analytical and Applied Pyrolysis,2012,97(5):116-122.
[2]聂发辉,刘荣荣,张慧敏,等.新型高级氧化技术处理硫化染料废水的研究进展[J].化工环保,2015,35(5):492-497.NIE F R,LIU R R,ZHANG H M,et al. Research progresses in treatment of sulfur dyes wastewater by new advanced oxidation technologies[J]. Environmental Protection of Chemical Industry,2015,35(5):492-497(in Chinese).
[3]李大培,刘玉春,华鹏,等.木质素基聚合物的制备及亚甲基蓝的吸附[J].化工环保,2016,32(2):173-178.LI D P,LIU Y C,HUA P,et al. Preparation of lignin-based polymer and adsorption of methylene blue[J]. Environmental Protection of Chemical Industry,2016,32(2):173-178(in Chinese).
[4] ABDELMJID B,MAJDA B,BRAHIM A,et al. Removal of dyes by a new nano-TiO2ultrafiltration membrane deposited on low-cost support prepared from natural Moroccan bentonite[J]. Applied Clay Science,2017,149:127-135.
[5]李庭,周成显怡,谢通慧,等. 4种触须式强碱性阴离子交换树脂的制备及其对曙红Y的吸附性能[J].化工进展,2015,34(5):1377-1388.LI T,ZHOU C X Y,XIE T H,et al. Preparation of four tentacle-type strong base anion exchange resins andstudy ontheir adsorption properties for Eosin Y removal[J]. Chemical Industry and Engineering Progress,2015,34(5):1377-1388(in Chinese).
[6]徐云兰,李珏秀,钟登杰,等.双极液膜法可见光光催化降解染料废水[J].中国环境科学,2014,34(6):1463-1470.XU Y L,Li Y X,Zhong D J,et al. Dual electrodes photocatalytic degradation of dye wastewater under visible light irradiation[J]. China Environmental Science,2014,34(6):1463-1470(in Chinese).
[7] LI X H,JIN X D,ZHAO N N,et al. Novel bio-electro-Fenton technology for azo dye wastewater treatment using microbial reverseelectrodialysis electrolysis cell[J]. Bioresource Technology,2017,228:322-329.
[8]张聪璐,胡筱敏,赵研,等.磁性壳聚糖衍生物对阴离子染料的吸附行为[J].环境科学,2015,36(1):221-226.ZHANG C L,HU X M,ZHAO Y,et al. Adsorption behavior of anionic dyes onto magnetic chitosan derivatives[J]. Environmental Science,2015,36(1):221-226(in Chinese).
[9] MA C F,GAO Q,XIA K S,et al. Three-dimensionally porous graphene:A high-performance adsorbent for removal of albumin-bonded bilirubin[J]. Colloids and Surfaces B:Biointerfaces,2017,149:146-153.
[10] QU Z,FANG L,CHEN D Y,et al. Effective and regenerable Ag/graphene adsorbent for Hg(Ⅱ)removal from aqueous solution[J].Fuel,2017,203:128-134.
[11] LIU Q,SHI J B,ZENG L X,et al. Evaluation of graphene as an advantageous adsorbent for solid-phase extraction with chlorophenols as model analytes[J]. Journal of Chromatography A,2010,1218(2):197-204.
[12] ZHANG L Y,ZHANG W L,ZHOU Z Q,et al.γ-Fe2O3nanocrystals-anchored macro/meso-porous graphene as a highly efficient adsorbent toward removal of methylene blue[J]. Journal of Colloid and Interface Science,2016,476:200-205.
[13] SAMIEE S,GOHARSHADI E K. Graphene nanosheets as efficient adsorbent for an azo dye removal:Kinetic and thermodynamic studies[J]. Journal of Nanoparticle Research,2014,16(8):2542-2557.
[14] SONG X H,LIN L P,RONG M C,et al. Mussel-inspired,ultralight,multifunctional 3d nitrogen-doped graphene aerogel[J]. Carbon,2014,80:174-182.
[15] CHENG C,DENG J,LEI B,et al. Toward 3d graphene oxide gels based adsorbents for high-efficient water treatment via the promotion of biopolymers[J]. Journal of Hazardous Materials,2013,263:467-478.
[16] LANGMUIR I. The adsorption of gases on plane surfaces of glass,mica and platinum[J]. Journal of the American Chemical Society,1918,40(9):1361-1403.
[17] CUI L M,WANG Y G,HU L H,et al. Mechanism of Pb(II)and methylene blue adsorption onto magnetic carbonate hydroxyapatite/graphene oxide[J]. RSC Advances,2015,5(3):9759-9770.
[18] SHI H C,LI W S,ZHONG L,et al. Methylene blue adsorption from aqueous solution by magnetic cellulose/graphene oxide composite:equilibrium,kinetics,and thermodynamics[J]. Industrial&Engineering Chemistry Research,2014,53(3):1108-1118.
[19] JIN L N,ZHAO X S,QIAN X Y,et al. Nickel nanoparticles encapsulated in porous carbon and carbon nanotube hybrids from bimetallic metal-organic-frameworks for highly efficient adsorption of dyes[J]. Journal of Colloid and Interface Science,2018,509:245-253.
[20] CHEN Y Q,CHEN L B,BAIH,et al. Graphene oxide-chitosan composite hydrogels as broad-spectrum adsorbents for water purification[J]. Journal of Materials Chemistry A,2013,1(6):1992-2001.
[21] WANG W,JIAO T F,ZHANG Q R,et al. Hydrothermal synthesis of hierarchical core-shell manganese oxide nanocomposites as efficient dye adsorbents for wastewater treatment[J]. RSC Advances,2015,5(69):56279-56285.
[22] GUO H Y,JIAO T F,ZHANG Q R,et al. Preparation of graphene oxide-based hydrogels as efficient dye adsorbents for wastewater treatment[J]. Nanoscale Research Letters,2015,10(1):272-281.
[23]常青,江国栋,胡梦璇,等.石墨烯基磁性复合材料吸附水中亚甲基蓝的研究[J].环境科学,2014,35(5):1804-1809.CHANG Q,JIANG G D,HU M X,et al. Adsorption of methylene blue from aqueous solution onto magnetic Fe3O4/graphene oxide nanoparticles[J]. Environmental Science,2014,35(5):1804-1809(in Chinese).
[24]邹禹涵.氧化石墨烯吸附亚甲基蓝的性能研究[J].佳木斯大学学报(自然科学版),2017,35(2):228-231.ZOU Y H. Study on the graphene oxide in adsorption of methylene blue[J]. Journal of Jiamusi University(Natural Science Edition),2017,35(2):228-231(in Chinese).
[25]吴艳,罗汉金,王侯,等.改性石墨烯对水中亚甲基蓝的吸附性能研究[J].环境科学,2013,34(11):4333-4340.WU Y,LUO H J,WANG H,et al. Adsorption properties of modified graphene for methylene blue removal fromwastewater[J].Environmental Science,2013,34(11):4333-4340(in Chinese).
[26]徐恩兵,李坤权,朱志强,等.双孔介孔碳的合成及其对亚甲基蓝的吸附[J].环境化学,2015,34(1):137-143.XU E B,LI K Q,ZHU Z Q,et al. Synthesis of mesoporous carbon with dual-pore structure and their adsorption of methylene blue[J].Environmental Chemistry,2015,34(1):137-143(in Chinese).
[27] YANG M L,LIU X L,QI Y C,et al. Preparation ofκ-carrageenan/graphene oxide gel beads and their efficient adsorption for methylene blue[J]. Journal of Colloid And Interface Science,2017,506:669-677.
[28] GUI C X,WANG Q Q,HAO S M,et al. Sandwichlike magnesium silicate/reduced graphene oxide nanocomposite for enhanced Pb2+and methylene blue adsorption[J]. ACS Applied Materials&Interfaces,2014,6(16):14653-14659.
[29] LIU C Y,LIU H Y,XU A R,et al. In situ reduced and assembled three-dimensional graphene aerogel for efficient dye removal[J].Journal of Alloys and Compounds,2017,714:522-529.
[30] THEYDAN S K,AHMED M J. Adsorption of methylene blue onto biomass-based activated carbon by Fe Cl3activation:Equilibrium,kinetics,and thermodynamic studies[J]. Journal of Analytical and Applied Pyrolysis,2012,97(5):116-122.