通过壳聚糖-g-N-羧甲基-2-硫代-4,5-2H咪唑啉酮(CTS-g-N-CSIDZ)非共价功能化多壁碳纳米管(MWCNTs)的方式制备固定漆酶载体,该复合物载体主要通过物理吸附和漆酶活性中心与载体上配体之间的配位作用来固定漆酶,较大程度地保持了游离漆酶活性位原始构象.将固定了漆酶的复合物附着在裸玻碳电极上便构筑了复合物固定漆酶修饰玻碳电极.在以分光光度法测定了这种复合物载体对漆酶的担载量、固定漆酶比活力、稳定性、重复使用性及其催化2,6-二甲氧基苯酚(DMP)氧化动力学参数的基础上,还对基于此种复合物固定漆酶修饰玻碳电极作为化学传感器(以DMP作为底物)的性能进行了研究.结果表明,该复合物具有较高的固酶担载量(81.7 mg/g)和固定漆酶比活力(1.33 U/mg)；而作为电化学传感器的复合物固定漆酶修饰玻碳电极对底物DMP具有较高的亲和力(对DMP的米氏常数KM是0.0918 mmol/L),较高的灵敏度( 3680 mA· L/mol),较低的检测限(3.3×10-4 mmol/L),较高的响应选择性,良好的重现性、重复使用性和长期稳定性.这种漆酶基电极有望用作电流型特定结构的酚类传感器.
参考文献
| [1] | Willner I,Yan Y M,Willner B,et al.Integrated Enzyme-based Biofuel Cells-A Review[J].Fuel Cells,2009,(1):17-24. |
| [2] | Ivannov I,Vidakovic-Koch T,Sundmacher K.Recent Advances in Enzymatic Fuel Cells:Experiments and Modelling[J].Energies,2010,(3):803-846. |
| [3] | 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. |
| [4] | 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. |
| [5] | Heller A.Miniature Biofuel Cells[J].P C C P,2004,(6):209-216. |
| [6] | Palmer A E,Randall D W,Xu F,et al.Spectroscopic Studies and Electronic Structure Description of the High Potential Type 1 Copper Site in Fungal Laccase:Insight into the Effect of the Axial Ligand[J].J Am Chem Soc,1999,121:7138-7149. |
| [7] | 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. |
| [8] | 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. |
| [9] | Qiu H J,Xu C X,Huang X R,et al.Immobilization of Laccase on Nanoporous Gold:Comparative Studies on the Immobilization Strategies and the Particle Size Effects[J].J Phys Chem C,2009,113(6):2521-2525. |
| [10] | Mano N,Mao F,Shin W,et al.A Miniature Biofuel Cell Operating at 0.78 V[J].Chem Commun,2003:518-519. |
| [11] | Zhu Y F,Kaskel S,Shi J L,et al.Immobilization of Trametes Versicolor Laccase on Magnetically Separable Mesoporous Silica Spheres[J].Chem Mater,2007,19:6408. |
| [12] | 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,2008,112:14781-14785. |
| [13] | Klis M,Karbarz M,Stojek Z,et al.Thermoresponsive Poly(N-Isopropylacry-lamide) Gel for Immobilization of Laccase on Indium Tin Oxide Electrodes[J].J Ph ys Chem B,2009,113:6062-6068. |
| [14] | Ackermann Y,Guschin D A,Eckhard K,et al.Design of a Bioelectrocatalytic Eectrode Interface for Oxygen Reduction in Biofuel Cells Based on A Specifically Adapted Os-Complex Containing Redox Polymer with Entrapped Trametes Hirsuta Laccase[J].Electrochem Commun,2010,12:640-643. |
| [15] | Mano N,Kim H H,Zhang Y C,et al.An Oxygen Cathode Operating in a Physiological Solution[J].J Am Chem Soc,2002,124:6480-6486. |
| [16] | Fei J F,Song H Y,Palmore G T R.A Biopolymer Composite That Catalyzes the Reduction of Oxygen to Water[J].Chem Mater,2007,19 (7):1565-1570. |
| [17] | Blanford C F,Heath R S,Armstrong F A.A Stable Electrode for High-potential,Electrocatalytic O2 Reduction Based on Rational Attachment of a Blue Copper Oxidase to a Graphite Surface[J].Chem Commun,2007:1710-1712. |
| [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] | Rahman M A,Noh H B,Shim Y B.Direct Electrochemistry of Laccase Immobilized on Au Nanoparticles EncapsulatedDendrimer Bonded Conducting Polymer:Application for a Catechin Sensor[J].Anal Chem,2008,80(21):8020-8027. |
| [21] | 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. |
| [22] | 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. |
| [23] | 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(11):1287-1291. |
| [24] | Liu J,Rinzler A G,Dai H J,et al.Fullerene Pipes[J].Science,1998,280:1253-1256. |
| [25] | HUANG Jun,ZHOU Juying,XIAO Haiyan,et al.Study of CuTAPc-Fe3 O4 Nanoparticles and Their Laccase[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. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%