Film-forming aminocellulose derivatives as enzyme-compatible support matrices for biosensor developments

被引:68
作者
Berlin, P
Klemm, D
Jung, A
Liebegott, H
Rieseler, R
Tiller, J
机构
[1] Forschungszentrum Julich, D-52425 Julich, Germany
[2] Univ Jena, Inst Organ Chem & Makromol Chem, D-07743 Jena, Germany
关键词
aminocellulose derivatives; atomic force microscopy; enzyme activity; enzyme coupling; GOD; HRP; LOD; nanostructures; stability; thin films;
D O I
10.1023/A:1027342027945
中图分类号
TB3 [工程材料学]; TS [轻工业、手工业、生活服务业];
学科分类号
0805 ; 080502 ; 0822 ;
摘要
Based on 6(2)-O-tosyl celluloses and 6(2)-O-tosylcellulose derivatives, it has been possible to synthesize a novel soluble aminocellulose type, P-CH2-NH-(X)-NH2 (P = cellulose, (X) = alkylene, aryl, aralkylene or oligoamine) with diamine or oligoamine residues at C6 and solubilizing groups (S) such as acetate, benzoate, carbanilate, methoxy and/or tosylate groups at C2/C3 of the anhydroglucose unit (AGU). Depending on the nature and degree of substitution (DS) of (S), the aminocelluloses are soluble either in DMA and DMSO or in water. They all form transparent films from their solutions. In the case of water-soluble aminocelluloses, for example, an enzyme-specific pH value can be adjusted by protonation of the NH2 end groups at C6. The aminocelluloses apparently form aggregates (on a scale of nanostructures) according to a structure-inherent organization principle. The nanostructures could be imaged on the aminocellulose film surface by atomic force microscopy (AFM) in the form of characteristic topographic structures - as a result of the aggregation of the aminocellulose derivative chains and their interaction with the functionalized film support. In this way, structural and environment-induced factors influencing the nanostructure formation were found. The aminocellulose films can be covalently coupled with biomolecules by bifunctional reaction via NH2-reactive compounds. With the aid of analytically relevant enzymes, e.g. glucose oxidase (GOD), horseradish peroxidase (HRP) and others, it was found that the enzyme parameters can be modified by the interplay of the aminocellulose and coupling structures. A number of new bifunctional enzyme coupling reactions, e.g. via L-ascorbic acid or benzenedisulfonyl chlorides, forming amide or sulfonamide coupling structures led to efficient enzyme activities and long-term stabilities in the case of GOD and HRP coupling to PDA cellulosetosylate films.
引用
收藏
页码:343 / 367
页数:25
相关论文
共 104 条
  • [1] THE DESIGN OF ENZYME SENSORS BASED ON THE ENZYME STRUCTURE
    ALVAREZICAZA, M
    KALISZ, HM
    HECHT, HJ
    AUMANN, KD
    SCHOMBURG, D
    SCHMID, RD
    [J]. BIOSENSORS & BIOELECTRONICS, 1995, 10 (08) : 735 - 742
  • [2] GLUCOSE-OXIDASE SANDWICHED BETWEEN PHEMA LAYERS - A CONTINUOUS-FLOW REACTOR APPLICATION
    ARICA, MY
    HASIRCI, V
    [J]. BIOMATERIALS, 1993, 14 (11) : 809 - 816
  • [3] BARMIN AV, 1993, BIOTECHNOL APPL BIOC, V18, P369
  • [4] BARTHEL H, 1996, ORGANOSILICON CHEM, V2, P765
  • [5] BECHER J, 2003, IN PRESS CELLULOSE
  • [6] Berlin P, 1998, PAPIER, V52, P737
  • [7] Berlin P, 2000, MACROMOL CHEM PHYSIC, V201, P2070, DOI 10.1002/1521-3935(20001001)201:15<2070::AID-MACP2070>3.0.CO
  • [8] 2-E
  • [9] BERLIN P, 1997, Patent No. 0873365
  • [10] BERLIN P, 2002, Patent No. 63587