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采用不同结构的高分子聚合物与纯化的多壁碳纳米管(MWCNTs)共混的方法,制备得到聚合物非共价功能化多壁碳管复合物,测定了这些载体对漆酶(lac)的担载量、固定漆酶的比活力及稳定性.以固定漆酶的复合物修饰玻碳(GC)电极后,采用循环伏安法研究这些电极在无氧磷酸盐缓冲液(PBS)中的直接电化学行为及催化氧还原活力,粗略地测定了固定漆酶与电极间电子转移的速率常数.实验结果表明,当聚合物中含亲漆酶基团或能与漆酶活性中心发生相互作用的官能团时利于直接电子转移,而且复合物固定漆酶保持了游离漆酶的天然构象.这些电极中,lac/NIPAM-co-BPCP-M WCNTs/GC(NIPAM-co-BPCP:N-烯丙基-1-苯甲酰基-3-苯基-4,5-2H-4-甲酰胺基吡唑-co-N-异丙基丙烯酰胺)在无氧PBS中发生直接电子转移的式电位(605mV)更接近漆酶活性中心的式电位(580mV),具有较快的异相电子转移速率(0.726s-1),较高的漆酶担载量(103.5mg/g)和固定漆酶比活力(1.68U/mg),较高的催化氧还原能力(氧还原起始电位820mV,在650mV时的催化峰电流为85.5μA)以及良好的重复使用性和长期使用性.

参考文献

[1] Willner I,Katz E,Chief-Edit.Bioelectronics[M].Chap 3.Strauss:Wiley-VCH,2005:35-93.
[2] Cracknell J A,Vincent K A,Armsrong F A.Enzymes as Working or Inspirational Electrocatalysts for Fuel Cells and Electrolysis[J].Chem Rev,2008,108:2439-2461.
[3] Yaropolov A I,Kharybin A N,Emneus J,et al.Flow-injection Analysis of Phenols at a Graphite Electrode Modified with co-Immobilised Laccase and Tyrosinase[J].Anal Chim Acta,1995,308:137-144.
[4] Jiang D S,Long S Y,Huang J,et al.Immobilization of Pycnoporus Sanguineus Laccase on Magnetic Chitosan Microspheres[J].Biochem Eng J,2005,25:15-23.
[5] Liu Y,Wang M K,Zhao F,et al.The Direct Electron Transfer of Glucose Oxidase and Glucose Biosensor Based on Carbon Nanotubes/Chitosan Matrix[J].Biosens Bioelectron,2005,21:984-988.
[6] Klis M,Karbarz M,Stojek Z,et al.Thermoresponsive Poly(N-Isopropylacrylamide) Gel for Immobilization of Laccase on Indium Tin Oxide Electrodes[J].J Phys Chem B,2009,113(17):6062-6068.
[7] Liu Y,Qu X H,Guo H W,et al.Facile Preparation of Amperometric Laccase Biosensor with Multifunction Based on the Matrix of Carbon Nanotubes-Chitosan Composite[J].Biosens Bioelectron,2006,21:2195-2201.
[8] Heller A.Miniature Biofuel Cells[J].Phys Chem Chem Phys,2004,6:209-216.
[9] Xiao Y,Patolsky F,Katz E,et al."Plugging into Enzymes":Nanowiring of Redox Enzymes by a Gold Nanoparticle[J].Science,2003,299:1877-1881.
[10] Willner I,Heleg-Shabtai V,Blonder R,et al.Electrical Wiring of Glucose Oxidase by Reconstitution of FAD-Modified Monolayers Assembled onto Au-Electrodes[J].J Am Chem Soc,1996,118(42):10321-10322.
[11] Qiu H J,Xu C X,Huang X R,et al.Adsorption of Laccase on the Surface of Nanoporous Gold and the Direct Electron Transfer between Them[J].J Phys Chem C,2008,112(38):14781-14785.
[12] Zheng W,Li Q F,Su L,et al.Direct Electrochemistry of Multi-Copper Oxidases at Carbon Nanotubes Noncovalently Functionalized with Cellulose Derivatives[J].Electroanalysis,2006,18(6):587-594.
[13] Rahman M A,Noh H B,Shim Y B.Direct Electrochemistry of Laccase Immobilized on Au Nanoparticles Encapsulated-Dendrimer Bonded Conducting Polymer:Application for a Catechin Sensor[J].Anal Chem,2008,80(21):8020-8027.
[14] Tsujimura S,Kamitaka Y,Kano K.Diffusional-Controlled Oxygen Reduction on Multi-Copper Oxidase-Adsorbed Carbon Aerogel Electrodes without Mediator[J].Fuel Cells,2007,6:463-469.
[15] Wen D,Xu X L,Dong S J.Single-Walled Carbon Nanohorn-based Miniature Glucose/Air Biofuel Cell for Harvesting Energy from Soft Drinks[J].Energy Environ Sci,2011,4:1358-1363.
[16] Santucci R,Ferri T,Morpurgo L,et al.Unmediated Heterogeneous Electron Transfer Reaction of Ascorbate Oxidase and Laccase at a Gold Electrode[J].Biochem J,1998,332:611-615.
[17] Shleev S,Christenson A,Serezhenkov V,et al.Electrochemical Redox Transformations of T1 and T2 Copper Sites in Native Trametes Hirsuta Laccase at Gold Electrode[J].Biochem J,2005,385:745-754.
[18] ZENG Han,ZHAO Shuxian,GONG Lanxin,et al.Immobilization of Laccase from Trametes Versicolor on the Matrix of N,N'-Methylene bis(acrylamide) Cross-linked Poly(methyl acrylic acid) and the Electrochemical Behavior of Its Modified Glassy Carbon Electrode[J].Chinese J Appl Chem,2010,27(9):1076-1082(in Chinese).曾涵,赵淑贤,龚兰新,等.云芝漆酶在N,N'-亚甲基双丙烯酰胺(BIS)交联聚甲基丙烯酸基元上的固定及其修饰玻碳电极电化学行为[J].应用化学,2010,27(9):1076-1082.
[19] ZENG Han,LIAO Lingwen,LI Mingfang,et al.Poly Aryl Amide and Carbon Nanotube Composite Supported Laccase Electrode and Its Electrochemical Behavior[J].Acta Phys Chim Sin,2010,26(12):3217-3224-(in Chinese).曾涵,廖铃文,李明芳,等.聚芳酰胺-多壁碳纳米管混合物固定漆酶电极的电化学行为[J].物理化学学报,2010,26(12):3217-3224.
[20] ZENG Han,ZHAO Shuxian,GONG Lanxin,et al.Direct Electrochemistry of Glassy Carbon Electrode Modified by Complex of Nanogold Sol and Chitosan-g-N-Carboxymethyl-Bi(2-Benzoimidazole)-1,2-Ethandiol with Laccase Entrapped[J].Chinese J Appl Chem,2011,28(3):326-332(in Chinese).曾涵,赵淑贤,龚兰新,等.壳聚糖-g-N-羧甲基-二(2-苯并咪唑)-1,2-乙二醇和纳米金溶胶复合物固定漆酶修饰玻碳电极的直接电化学[J].应用化学,2011,28(3):326-332.
[21] ZENG Han,ZHAO Shuxian,XU Jiangling,et al.Preparation of Chitosan-g-N-carboxy-methyl-2-sulfo-4,5-2H Imidazolinone and Its Antibacterial Behavior[J].Chinese J Appl Chem,2009,26(11):1287-1291(in Chinese).曾涵,赵淑贤,徐江玲,等.壳聚糖-g-N-羧甲基-2-硫代-4,5-2H咪唑啉酮的制备及其抑菌性能[J].应用化学,2009,26(ll):1287-1291.
[22] ZENG Han,ZHAO Shuxian,LI Yawei.Corrosion Inhibition and Antibacterial Effects of Copolymer NIPAM-co-BPCP on N80 Steel Panel[J].Chinese J Appl Chem,2010,27(4):478-483(in Chinese).曾涵,赵淑贤,李亚薇.N-异丙基丙烯酰胺与N-烯丙基-1-苯甲酰基-3-苯基-4,5-2H-4-甲酰胺基吡唑共聚物对N80钢片的化学和细菌腐蚀的抑制作用[J].应用化学,2010,27(4):478-483.
[23] ZENG Han,ZHAO Shuxian,WANG Yongjiang,et al.Synthesis of 3,4-Diolthiophene-2,5-bis Carbonyl Cross-linked Chitosan and Its Application as Antibacterial Reagent for Preserving White Peach[J].Chinese J Appl Chem,2010,27(11):1265-1271(in Chinese).曾涵,赵淑贤,王永疆,等.3,4-二羟基噻吩交联壳聚糖的合成及其对白桃的抑菌保鲜性能[J].应用化学,2010,27(11):1265-1271.
[24] LIU Li.Study of Phthaloylation of Chitosan and Their Graft Modification[D].Hefei:University of Science and Technology of China,2005(in Chinese).刘黎.壳聚糖的邻苯二甲酰化及其接枝改性的研究[D].合肥:中国科学技术大学,2005.
[25] Liu J,Rinzler A G,Dai H J,et al.Fullerene Pipes[J].Science,1998,280:1253-1256.
[26] HUANG Jun,ZHOU Juying,XIAO Haiyan,et al.Study of CuTAPc-Fe3O4 Nanoparticles and Their Laccase Immobilization[J].Acta Chim Sin,2005,63(14):1343-1347(in Chinese).黄俊,周菊英,肖海燕,等.CuTAPc-Fe3O4纳米复合粒子及其漆酶固定化研究[J].化学学报,2005,63(14):1343-1347.
[27] ZENG Han,YIN Xiaoli,YANG Zhongli,et al.Immobilization Approaches of Laccase on Nanogold Sol/Multi-walled Carbon Nanotube Matrices and the Particle Size Effects[J].Chinese J Appl Chem,2010,27(7):829-835(in Chinese).曾涵,尹筱莉,杨忠丽,等.漆酶在纳米金溶胶/多重壁碳纳米管复合载体上固定方法的比较及粒子尺寸效应[J].应用化学,2010,27(7):829-835.
[28] Shleev S,Kasmi A E,Ruzgas T,et al.Direct Heterogeneous Electron Transfer Reactions of Bilirubin Oxidase at A Spectrographic Graphite Electrode[J].Electrochem Commun,2004,(6):934-939.
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