[1]薛蓓,房伶晏,梁辰,等.磁性木质素制备及其对染料的吸附性能[J].林业工程学报,2019,4(04):85-92.[doi:10.13360/j.issn.2096-1359.2019.04.013]
 XUE Bei,FANG Lingyan,LIANG Chen,et al.Preparation of lignin/Fe3O4 based magnetic material and their performance in adsorption of dyes[J].Journal of Forestry Engineering,2019,4(04):85-92.[doi:10.13360/j.issn.2096-1359.2019.04.013]
点击复制

磁性木质素制备及其对染料的吸附性能()
分享到:

《林业工程学报》[ISSN:1001-8081/CN:32-1160/S]

卷:
4
期数:
2019年04期
页码:
85-92
栏目:
生物质能源与材料
出版日期:
2019-07-09

文章信息/Info

Title:
Preparation of lignin/Fe3O4 based magnetic material and their performance in adsorption of dyes
文章编号:
2096-1359(2019)04-0085-08
作者:
薛蓓13房伶晏13梁辰2李鑫13赖晨欢13勇强13黄曹兴123*
1.南京林业大学,江苏省林业资源高效加工利用协同创新中心,南京 210037; 2.广西清洁化制浆造纸与污染控制重点实验室,南宁 530004; 3.南京林业大学化学工程学院,南京 210037
Author(s):
XUE Bei13 FANG Lingyan13 LIANG Chen2 LI Xin13 LAI Chenhuan13 YONG Qiang13 HUANG Caoxing123*
1.Jiangsu Co-Innovation Center for Efficient Processing and Utilization of Forest Resources, Nanjing Forestry University, Nanjing 210037, China; 2.Guangxi Key Laboratory of Clean Pulp & Papermaking and Pollution Control, Nanning 530004, China; 3.Colle
关键词:
木质素 磁性木质素 Fe3O4 磁学性能 染料吸附
Keywords:
lignin magnetic lignin Fe3O4 magnetic property dyes adsorption
分类号:
TQ35
DOI:
10.13360/j.issn.2096-1359.2019.04.013
文献标志码:
A
摘要:
纳米材料粒径小、比表面积大、表面能高,具有良好的吸附特性。以磁性纳米颗粒合成的材料作为吸附材料时,不仅表现出高吸附容量,且易于回收和循环使用。本研究以沉淀法合成的超顺磁性Fe3O4纳米颗粒为负载物质,以黑液木质素为载体,采用原位吸附法和氨丙基三乙氧基硅烷(APTES)交联法分别制备磁性木质素Fe3O4@木质素和Fe3O4@APTES@木质素。采用红外线光谱仪、X射线衍射仪、透射电子显微镜、扫描电镜和振动样品磁强计对磁性木质素进行分析表征,并考察这些磁性木质素对染料(亚甲基蓝、刚果红和甲基橙)的吸附性能。结果显示:通过原位吸附法和交联法均能使木质素负载在Fe3O4外层,形成的Fe3O4@木质素和Fe3O4@APTES@木质素具有核壳结构,饱和磁强度分别为51和22 emu/g,负载前后Fe3O4的晶型结构和木质素的分子结构均不受影响。与黑液木质素、Fe3O4@木质素相比,利用交联法得到的Fe3O4@APTES@木质素对染料吸附性能最好,在颗粒添加量1.5 g/L,吸附温度298 K,初始染料质量浓度100 mg/L条件下,亚甲基蓝、刚果红和甲基橙的最大吸附量分别达到140.2,181.4和71.2 mg/g,吸附后磁性木质素在外磁场作用下能够从体系中分离出来,回收过程简便。
Abstract:
Nanomaterial has the properties of small particle size, large specific surface area and high surface energy, which make it an excellent candidate as the adsorbent.Introducing magnetic ability to nano-adsorbentcan facilitate the recovery and recycling of the nano-adsorbent.Although lignin has be used as the adsorbent to adsorb the dyes of methylene blue, congo red and methyl orange, it is non-recyclable and has limit adsorption capacity.In this study, magnetic nano-adsorbent was prepared from super paramagnetic nanoparticles of Fe3O4 and lignin precipitated from black liquor by in situ adsorption method and aminopropyltriethoxysilane cross-linking method.The resulted magnetic lignin/Fe3O4 based materials were termed as Fe3O4@lignin and Fe3O4@APTES@lignin, respectively.The as-synthesized magnetic lignins Fe3O4@lignin and Fe3O4@APTES@lignin were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, transmission electron microscopy, scanning electron microscopy and vibrating sample magnetometerto understand their chemical and physical properties.Meanwhile, the adsorption performance of magnetic lignins on methylene blue, congo red and methyl orange were investigated.The results showed that lignins could successfully load on the surface of the Fe3O4 particles through both in situ adsorption method and aminopropyltriethoxysilane cross-linking method.The synthesized Fe3O4@lignin and Fe3O4@APTES@lignin exhibited a core-shell structures with the saturation magnetic intensity of 51 and 22 emu/g, respectively.In addition, it is found that the crystal structure of Fe3O4 particles and molecular structure of lignin were not changed in the synthesized magnetic lignins.Under the adsorption conditions of 1.5 g/L particle addition, 298 K, and dye concentration with 100 mg/L,Fe3O4@APTES@lignin showed the maximal adsorption capacity to adsorb methylene blue, congo red and methyl orange of 140.2, 181.4, and 71.2 mg/g, respectively.After adsorption, the magnetic lignins could be easily separated and recovered by a magnet.

参考文献/References:

[1] 韩秀丽, 郭晓锋, 王铎, 等.木质素基活性炭对刚果红的吸附性能研究[J].应用化工, 2016, 45(10):1903-1907.DOI:10.16581/j.cnki.issn1671-3206.2016.0705.046.
HAN X L, GUO X F, WANG D, et al.Study on the adsorption characteristics of Congo red by lignin-based activated carbon[J].Applied Chemical Industry, 2016, 45(10):1903-1907.
[2] 魏亮, 陈小光, 黄波, 等.偶氮染料废水厌氧生物脱色强化[J].纺织学报, 2018, 39(8):83-87.DOI:10.13475/j.fzxb.20170802405.
WEI L, CHEN X G, HUANG B, et al.Enhancement on anaerobic biological decoloration of azo dyes wastewater[J].Journal of Textile Research, 2018, 39(8):83-87.
[3] CHEQUER F M D, LIZIER T M, DE FELÍCIO R, et al.The azo dye Disperse Red 13 and its oxidation and reduction products showed mutagenic potential[J].Toxicology in Vitro, 2015, 29(7): 1906-1915.DOI:10.1016/j.tiv.2015.08.001.
[4] ROYER B, CARDOSO N F, LIMA E C, et al.Organofunctionalized kenyaite for dye removal from aqueous solution[J].Journal of Colloid and Interface Science, 2009, 336(2):398-405.DOI:10.1016/j.jcis.2009.04.025.
[5] XU W J, ZHANG W S, LI W, et al.Synthesis of poly(vinyl acetate)by degenerative transfer polymerization in the presence of iodine[J].Journal of Applied Polymer Science, 2012, 126(1): 104-109.DOI:10.1002/app.36664.
[6] YOU H, CHEN J C, YANG C, et al.Selective removal of cationic dye from aqueous solution by low-cost adsorbent usingphytic acid modified wheat straw[J].Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2016, 509: 91-98.DOI:10.1016/j.colsurfa.2016.08.085.
[7] 王犇, 朱现波.木质素基磁性炭的制备工艺优化[J].青岛科技大学学报(自然科学版), 2017, 38(4):12-18.DOI: 10.16351/j.1672-6987.2017.04.002.
WANG B, ZHU X B.Optimization of preparation technology of lignin-based magnetic carbon[J].Journal of Qingdao University of Science and Technology(Natural Science Edition), 2017, 38(4):12-18.
[8] DO M H, PHAN N H, NGUYEN T D, et al.Activated carbon/Fe3O4 nanoparticle composite: fabrication, methyl orange removal and regeneration by hydrogen peroxide[J].Chemosphere, 2011, 85(8):1269-1276.DOI:10.1016/j.chemosphere.2011.07.023.
[9] 徐鹏, 梁旭光, 曹小勇, 等.Fe3O4@SiO2@PAA多层核-壳结构复合微球的制备及吸附染料研究[J].林业工程学报, 2018, 3(3):52-56.DOI:10.13360/j.issn.2096-1359.2018.03.009.
XU P, LIANG X G,CAO X Y, et al.Preparation of Fe3O4@SiO2@PAA multilayer core-shell structural composite microspheres and its dye adsorption performance[J].Journal of Forestry Engineering, 2018, 3(3):52-56.
[10] YANG L J, ZHANG YY, LIU X Y, et al.The investigation of synergistic and competitive interaction between dye Congo red and methyl blue on magnetic MnFe2O4[J].Chemical Engineering Journal, 2014, 246:88-96.DOI:10.1016/j.cej.2014.02.044.
[11] 黄曹兴, 何娟, 赖晨欢, 等.毛竹预处理黑液木质素和酶解木质素的结构与热学性质[J].林业科学, 2018, 54(3):108-116.DOI:10.11707/j.1001-7488.20180311.
HUANG C X, HE J, LAI C H, et al.Structure characteristics and thermal properties of black liquor lignin and enzymatic hydrolysis lignin from moso bamboo pretreated by kraft pulping[J].Scientia Silvae Sinicae, 2018, 54(3):108-116.
[12] 许文静, 张文生, 李焱, 等.木质素磺酸钙改性丙烯酸树脂对水中甲基橙的吸附研究[J].高分子学报, 2016, 3(3):307-314.DOI:10.11777/j.issn1000-3304.2016.15194.
XU W J, ZHANG W S, LI Y, et al.Adsorption of methyl orange dye from aqueous solutions by acrylic composite resin chemically modified with calcium lignosulphonate[J].Acta Polymerica Sinica, 2016, 3(3):307-314.
[13] HUANG C X, HE J, NARRON R, et al.Characterization ofkraft lignin fractions obtained by sequential ultrafiltration and their potential application as a biobased component in blends with polyethylene[J].ACS Sustainable Chemistry & Engineering, 2017, 5(12):11770-11779.DOI:10.1021/acssuschemeng.7b03415.
[14] 黄曹兴, 何娟, 闵斗勇, 等.稀硫酸预处理对毛竹竹黄木质素结构的影响[J].林业工程学报, 2016, 1(1):55-60.DOI:10.13360/j.issn.2096-1359.2016.01.011.
HUANG C X, HE J, MIN D Y, et al.Effect of dilute acid pretreatment on the lignin structure of Moso bamboo inner skin[J].Journal of Forestry Engineering, 2016, 1(1):55-60.
[15] 冯斌, 任志强, 屈晶苗, 等.3-氨丙基三乙氧基硅烷表面修饰的磁性Fe3O4纳米粒子合成与表征[J].化工新型材料, 2008, 36(12):26-29.DOI:10.3969/j.issn.1006-3536.2008.12.009.
FENG B, REN Z Q, QU J M, et al.Preparation and characterization of(3-aminopropyl)triethoxysilane coated magnetite nanoparticles[J].New Chemical Materials, 2008, 36(12):26-29.
[16] 娄志超, 韩贺, 杨淋添, 等.木质复合磁性板材的制备及其电磁波吸收性能[J].林业工程学报, 2018, 3(6):25-31.DOI:10.13360/j.issn.2096-1359.2018.06.004.
LOU Z C, HAN H, YANG L T, et al.Preparation of multi-layer magnetic board, and its electromagnetic wave shielding properties[J].Journal of Forestry Engineering, 2018, 3(6):25-31.
[17] 琚彩霞, 徐甲坤, 张权, 等.氨基硅烷化磁性纳米微球的制备及性能研究[J].中国海洋大学学报, 2013, 43(11):71-76.DOI:10.16441/j.cnki.hdxb.2013.11.010.
JU C X, XU J K, ZHANG Q, et al.Preparation of aminosilane modified magnetic nanomicrospheres and its performance study[J].Periodical of Ocean University of China, 2013, 43(11):71-76.
[18] 顾银君, 王秀玲, 陈恭, 等.氨基硅烷化磁性纳米粒子的制备与表征[J].苏州科技学院学报(自然科学版), 2012, 29(1):42-46.DOI:10.3969/j.issn.1672-0687.2012.01.010.
GU Y J, WANG X L, CHEN G, et al.Synthesis and characterization of magnetic nanoparticles modified by 3-aminopropyltriethoxy-silane[J].Journal of Suzhou University of Science and Technology(Natural Science), 2012, 29(1):42-46.
[19] MIKHAYLOVA M, KIM D K, BOBRYSHEVA N, et al.Superparamagnetism of magnetite nanoparticles: dependence on surface modification[J].Langmuir, 2004, 20(6):2472-2477.DOI:10.1021/la035648e.
[20] DEATSCH A E, EVANS B A.Heating efficiency in magnetic nanoparticle hyperthermia[J].Journal of Magnetism and Magnetic Materials, 2014, 354:163-172.DOI:10.1016/j.jmmm.2013.11.006.
[21] 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, 36(2):173-178.DOI:10.3969/j.issn.1006-1878.2016.02.010.
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, 36(2):173-178.
[22] COTORUELO L M, MARQUÉS M D, DÍAZ F J, et al.Equilibrium and kinetic study ofcongo red adsorption onto lignin-based activated carbons[J].Transport in Porous Media, 2010, 83(3): 573-590.DOI:10.1007/s11242-009-9460-8.
[23] 苗天博, 陈葓, 刘明华.氰乙基球形木质素吸附剂对亚甲基蓝的吸附行为研究[J].中国造纸学报, 2015, 30(1):40-45.DOI:10.11981/j.issn.1000-6842.2015.01.40.
MIAO T B, CHEN H, LIU M H.Adsorption behavior of methylene blue on cyanoethyl spherical lignin adsorbent[J].Transactions of China Pulp and Paper, 2015, 30(1):40-45.
[24] ALBADARIN A B, COLLINS M N, NAUSHAD M, et al.Activated lignin-chitosan extruded blends for efficient adsorption of methylene blue[J].Chemical Engineering Journal, 2017, 307: 264-272.DOI:10.1016/j.cej.2016.08.089.
[25] 李萌.阳离子型木质素基水凝胶的制备及其在废水处理中的应用[D].济南: 齐鲁工业大学, 2016.
LI M.Preparation of cationic lignin-based hydrogels and its application in wastewater treatment[D].Jinan: Qilu University of Technology, 2016.

相似文献/References:

[1]徐旭东,洪枢,安然,等.低共熔离子液体中氯化钯催化改性木质素的结构特征[J].林业工程学报,2015,29(06):116.[doi:10.13360/j.issn.1000-8101.2015.06.029]
 XU Xu-dong,HONG Shu,AN Ran,et al.Structural features of lignin modified by palladium chloride catalyst in eutectic ionic liquids[J].Journal of Forestry Engineering,2015,29(04):116.[doi:10.13360/j.issn.1000-8101.2015.06.029]
[2]王翔,蒋帅南,陈敏智,等.木质素基碳纤维研究进展[J].林业工程学报,2016,1(01):83.[doi:10.13360/j.issn.2096-1359.2016.01.016]
 WANG Xiang,JIANG Shuainan,CHEN Minzhi,et al.Review of research progress on lignin-based carbon fibers[J].Journal of Forestry Engineering,2016,1(04):83.[doi:10.13360/j.issn.2096-1359.2016.01.016]
[3]李伟,佟国宾△,王梦茹,等.碱木质素基碳量子点/TiO2复合光催化剂的制备[J].林业工程学报,2016,1(05):84.[doi:10.13360/j.issn.2096-1359.2016.05.015]
 LI Wei,TONG Guobin,WANG Mengru,et al.Preparation of the alkaline lignin pyrolytic based carbon quantum dots/TiO2 composite photocatalyst[J].Journal of Forestry Engineering,2016,1(04):84.[doi:10.13360/j.issn.2096-1359.2016.05.015]
[4]王飞,吴真,张军,等.木质素原料制备烃类化合物的研究进展[J].林业工程学报,2017,2(03):1.[doi:10.13360/j.issn.2096-1359.2017.03.001]
 WANG Fei,WU Zhen,ZHANG Jun,et al.Advances in production of hydrocarbon compounds from lignin[J].Journal of Forestry Engineering,2017,2(04):1.[doi:10.13360/j.issn.2096-1359.2017.03.001]
[5]刘源松,关明杰*,张志威,等.木质素改性脲醛树脂对竹层积材甲醛释放量及胶合性能的影响[J].林业工程学报,2017,2(03):28.[doi:10.13360/j.issn.2096-1359.2017.03.005]
 LIU Yuansong,GUAN Mingjie*,ZHANG Zhiwei,et al.Effect of lignin modified urea-formaldehyde resin on the formaldehyde emission and bonding performance of bamboo laminated timber[J].Journal of Forestry Engineering,2017,2(04):28.[doi:10.13360/j.issn.2096-1359.2017.03.005]
[6]张学铭,吴苗,许凤*.木质素化学催化解聚研究新进展[J].林业工程学报,2017,2(04):1.[doi:10.13360/j.issn.2096-1359.2017.04.001]
 ZHANG Xueming,WU Miao,XU Feng*.Recent development on conversion of lignin into aromatics based on catalytical depolymerization[J].Journal of Forestry Engineering,2017,2(04):1.[doi:10.13360/j.issn.2096-1359.2017.04.001]
[7]文甲龙,陈天影,孙润仓*.生物质木质素分离和结构研究方法进展[J].林业工程学报,2017,2(05):76.[doi:10.13360/j.issn.2096-1359.2017.05.014]
 WEN Jialong,CHEN Tianying,SUN Runcang*.Research progress on separation and structural analysis of lignin in lignocellulosic biomass[J].Journal of Forestry Engineering,2017,2(04):76.[doi:10.13360/j.issn.2096-1359.2017.05.014]
[8]应文俊,吴凯,赵存异,等.碱木质素聚乙氧基接枝共聚物表面特性对纤维素酶糖化效率的影响[J].林业工程学报,2018,3(04):68.[doi:10.13360/j.issn.2096-1359.2018.04.012]
 YING Wenjun,WU Kai,ZHAO Cunyi,et al.Effect of surface property of polyoxyethylene ether grafted alkali lignin on saccharification of Avicel[J].Journal of Forestry Engineering,2018,3(04):68.[doi:10.13360/j.issn.2096-1359.2018.04.012]
[9]黄曹兴,何娟,梁辰,等.木质素的高附加值应用研究进展[J].林业工程学报,2019,4(01):17.[doi:10.13360/j.issn.2096-1359.2019.01.003]
 HUANG Caoxing,HE Juan,LIANG Chen,et al.Progress in applications of high value-added lignin materials[J].Journal of Forestry Engineering,2019,4(04):17.[doi:10.13360/j.issn.2096-1359.2019.01.003]
[10]程承,陶桂祥,王琦,等.木质素改性沥青高温性能试验[J].林业工程学报,2019,4(01):141.[doi:10.13360/j.issn.2096-1359.2019.01.021]
 CHENG Cheng,TAO Guixiang,WANG Qi,et al.Experimental study on performance of lignin-modified asphalt at high temperatures[J].Journal of Forestry Engineering,2019,4(04):141.[doi:10.13360/j.issn.2096-1359.2019.01.021]

备注/Memo

备注/Memo:
收稿日期:2018-12-08 修回日期:2019-03-19
基金项目:国家自然科学基金青年基金项目(31800501); 江苏省自然科学基金青年基金项目(BK20180772); 广西清洁化制浆造纸与污染控制重点实验室开放基金资助(KF 201725)。
作者简介:薛蓓,女,研究方向为生物工程。通信作者:黄曹兴,男,讲师。E-mail:hcx@njfu.edu.cn
更新日期/Last Update: 2019-07-10