Enzyme immobilization on silane-modified surface through short linkers: fate of interfacial phases and impact on catalytic activity

Langmuir. 2014 Apr 15;30(14):4066-77. doi: 10.1021/la404935q. Epub 2014 Apr 2.

Abstract

We investigated the mechanism of enzyme immobilization on silanized surfaces through coupling agents (cross-linkers) in order to understand the role of these molecules on interfacial processes and their effect on catalytic activity. To this end, we used a model multimeric enzyme (G6PDH) and several cross-linking molecules with different chemical properties, including the nature of the end-group (-NCO, -NCS, -CHO), the connecting chain (aliphatic vs aromatic), and geometrical constraints (meta vs para-disubstituted aromatics). There did not seem to be radical differences in the mechanism of enzyme adsorption according to the linker used as judged from QCM-D, except that in the case of DIC (1,4-phenylene diisocyanate) the adsorption occurred more rapidly. In contrast, the nature of the cross-linker exerted a strong influence on the amount of enzyme immobilized as estimated from XPS, and more unexpectedly on the stability of the underlying silane layer. DIC, PDC (1,4-phenylene diisothiocyanate), or GA (glutaraldehyde) allowed successful enzyme immobilization. When the geometry of the linker was changed from 1,4-phenylene diisothiocyanate to 1,3-phenylene diisothiocyanate (MDC), the silane layer was subjected to degradation, upon enzyme adsorption, and the amount of immobilized molecules was significantly lowered. TE (terephtalaldehyde) and direct enzyme deposition without cross-linker were similar to MDC. The organization of immobilized enzymes also depended on the immobilization procedure, as different degrees of aggregation were observed by AFM. A correlation between the size of the aggregates and the catalytic properties of the enzyme was established, suggesting that aggregation may enhance the thermostability of the multimeric enzyme, probably through a compaction of the 3D structure.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Biocatalysis
  • Cross-Linking Reagents / chemistry
  • Cross-Linking Reagents / metabolism
  • Enzymes, Immobilized / chemistry
  • Enzymes, Immobilized / metabolism*
  • Glucosephosphate Dehydrogenase / chemistry
  • Glucosephosphate Dehydrogenase / metabolism*
  • Particle Size
  • Silanes / chemistry
  • Silanes / metabolism*
  • Surface Properties

Substances

  • Cross-Linking Reagents
  • Enzymes, Immobilized
  • Silanes
  • Glucosephosphate Dehydrogenase