Novel multienzyme oxidative biocatalyst for lignin bioprocessing.

A novel multienzyme biocatalyst, based on coimmobilization of the laccase and horseradish peroxidase by cross linking and layer-by-layer coating with polyelectrolyte, was designed, synthesized and applied at the development of an oxidative cascade process on lignin. The efficiency and specificity of the new LbL-multienzyme system, the occurrence of a synergy of the co-immobilized enzymes, the lignin oxidation pathway and the nature of the structural modifications occurred in treated lignins have been investigated in the present effort by means of GPC analysis and quantitative (31)P NMR techniques.

[1]  U. Hanefeld,et al.  Carrier enabled catalytic reaction cascades. , 2006, Chemical communications.

[2]  C. Collins,et al.  Immobilization of horseradish peroxidase onto polyaniline polymers , 2003 .

[3]  N. C. Veitch,et al.  Horseradish peroxidase: a modern view of a classic enzyme. , 2004, Phytochemistry.

[4]  R. Willson,et al.  Radical-cations as reference chromogens in kinetic studies of ono-electron transfer reactions: pulse radiolysis studies of 2,2′-azinobis-(3-ethylbenzthiazoline-6-sulphonate) , 1982 .

[5]  J. Hajdu,et al.  The catalytic pathway of horseradish peroxidase at high resolution , 2002, Nature.

[6]  Lucia Gardossi,et al.  Understanding enzyme immobilisation. , 2009, Chemical Society reviews.

[7]  C. Crestini,et al.  A novel and efficient oxidative functionalization of lignin by layer-by-layer immobilised Horseradish peroxidase. , 2011, Bioorganic & medicinal chemistry.

[8]  D. Argyropoulos.  Quantitative phosphorus-31 NMR analysis of lignins, a new tool for the lignin chemist , 1994 .

[9]  S. S. Narayanan,et al.  Fabrication of bienzyme nanobiocomposite electrode using functionalized carbon nanotubes for biosensing applications. , 2008, Biosensors & bioelectronics.

[10]  José M Pingarrón,et al.  Integrated multienzyme electrochemical biosensors for monitoring malolactic fermentation in wines. , 2010, Talanta.

[11]  A. Mayer,et al.  Laccase: new functions for an old enzyme. , 2002, Phytochemistry.

[12]  Roger A Sheldon,et al.  E factors, green chemistry and catalysis: an odyssey. , 2008, Chemical communications.

[13]  G. Henriksson,et al.  Oxidative polymerisation of models for phenolic lignin end-groups by laccase , 2009 .

[14]  S. Campuzano,et al.  Integrated multienzyme electrochemical biosensors for the determination of glycerol in wines. , 2008, Analytica chimica acta.

[15]  C. Crestini,et al.  Oxidative strategies in lignin chemistry: A new environmental friendly approach for the functionalisation of lignin and lignocellulosic fibers , 2010 .

[16]  T. Tzanov,et al.  An acid-stable laccase from Sclerotium rolfsii with potential for wool dye decolourization , 2003 .

[17]  C. Crestini,et al.  The Immobilized Porphyrin‐Mediator System Mn(TMePyP)/clay/HBT (clay‐PMS): A Lignin Peroxidase Biomimetic Catalyst in the Oxidation of Lignin and Lignin Model Compounds , 2004 .

[18]  D. Argyropoulos.  31P NMR in wood chemistry: A review of recent progress , 1995 .

[19]  N. Durán,et al.  Effluent Treatment of Pulp and Paper, and Textile Industries using Immobilised Horseradish Peroxidase , 1998 .

[20]  J. Toca-Herrera,et al.  Efficiency of a bienzyme sequential reaction system immobilized on polyelectrolyte multilayer-coated colloids. , 2008, Langmuir : the ACS journal of surfaces and colloids.

[21]  J. Bailey,et al.  Immobilization of enzymes on activated carbon: Selection and preparation of the carbon support , 1979, Biotechnology and bioengineering.

[22]  Johannes Schmitt,et al.  Fine-Tuning of the film thickness of ultrathin multilayer films composed of consecutively alternating layers of anionic and cationic polyelectrolytes , 1992 .

[23]  M. Galbe,et al.  Reduced inhibition of enzymatic hydrolysis of steam-pretreated softwood. , 2001, Enzyme and microbial technology.

[24]  K. E. Everse,et al.  Peroxidases in chemistry and biology , 1990 .

[25]  H. Jia,et al.  Enabling multienzyme biocatalysis using nanoporous materials , 2004, Biotechnology and bioengineering.

[26]  C. Crestini,et al.  SINGLET OXYGEN IN THE PHOTODEGRADATION OF LIGNIN MODELS , 1997 .

[27]  Ting Chen,et al.  A novel immobilization multienzyme glucose fluorescence capillary biosensor. , 2010, Biosensors & bioelectronics.

[28]  A. J. Augustine,et al.  Spectroscopic studies of perturbed T1 Cu sites in the multicopper oxidases Saccharomyces cerevisiae Fet3p and Rhus vernicifera laccase: allosteric coupling between the T1 and trinuclear Cu sites. , 2008, Biochemistry.

[29]  T. Tzanov,et al.  Immobilization of catalases from Bacillus SF on alumina for the treatment of textile bleaching effluents. , 2001, Enzyme and microbial technology.

[30]  C. McNeil,et al.  Disposable tyrosinase-peroxidase bi-enzyme sensor for amperometric detection of phenols. , 2002, Biosensors & bioelectronics.

[31]  C. Crestini,et al.  Oxidative functionalisation of lignin by layer-by-layer immobilised laccases and laccase microcapsules , 2010 .

[32]  Charlotte Carlsson,et al.  Amperometric screen-printed biosensor arrays with co-immobilised oxidoreductases and cholinesterases , 2005 .

[33]  Elio Santacesaria,et al.  Lactose hydrolysis by immobilized β-galactosidase: the effect of the supports and the kinetics , 2003 .

[34]  Stephen Y. Lin,et al.  Methods in Lignin Chemistry , 1992, Springer Series in Wood Science.

[35]  C. Crestini,et al.  On the mechanism of the laccase-mediator system in the oxidation of lignin. , 2003, Chemistry.

[36]  Jenny Emnéus,et al.  Peroxidase-modified electrodes: Fundamentals and application , 1996 .

[37]  A. Yaropolov,et al.  Laccase: properties, catalytic mechanism, and applicability , 1994 .

[38]  B. Krajewska.  Application of chitin- and chitosan-based materials for enzyme immobilizations: a review , 2004 .

[39]  Ana M Azevedo,et al.  Horseradish peroxidase: a valuable tool in biotechnology. , 2003, Biotechnology annual review.

[40]  Gero Decher,et al.  Fuzzy Nanoassemblies: Toward Layered Polymeric Multicomposites , 1997 .

[41]  R. Kessler,et al.  Study of dye decolorization in an immobilized laccase enzyme‐reactor using online spectroscopy , 2004, Biotechnology and bioengineering.

[42]  Lu,et al.  The DFRC Method for Lignin Analysis. 2. Monomers from Isolated Lignins. , 1998, Journal of agricultural and food chemistry.

[43]  J. Buchert,et al.  Oxidation of milled wood lignin with laccase, tyrosinase and horseradish peroxidase , 2005, Applied Microbiology and Biotechnology.

[44]  J. Cabral,et al.  Operational stability of immobilised horseradish peroxidase in mini-packed bed bioreactors , 2004 .

[45]  K. Welinder.  Superfamily of plant, fungal and bacterial peroxidases , 1992 .

[46]  L. Bachas,et al.  Controlled layer-by-layer immobilization of horseradish peroxidase. , 1999, Biotechnology and bioengineering.

[47]  M. M. Bradford.  A rapid and sensitive method for the quantitation of microgram quantities of protein utilizing the principle of protein-dye binding. , 1976, Analytical biochemistry.

[48]  Roger A. Sheldon,et al.  Enzyme Immobilization: The Quest for Optimum Performance , 2007 .

[49]  S. R. Couto,et al.  Coating of immobilised laccase for stability enhancement: A novel approach , 2007 .

[50]  Lars Dähne,et al.  Tailor-made polyelectrolyte microcapsules: from multilayers to smart containers. , 2004, Angewandte Chemie.

[51]  Fang Wang,et al.  Fiber optic biosensors for hydrogen peroxide and L-lactate , 1995, Other Conferences.

[52]  J. Pingarrón,et al.  Composite Multienzyme Amperometric Biosensors for an Improved Detection of Phenolic Compounds , 2003 .

[53]  C. Crestini,et al.  Structural modifications induced during biodegradation of wheat lignin by Lentinula edodes. , 1998, Bioorganic & medicinal chemistry.

[54]  Sung-Chyr Lin,et al.  Application of immobilized horseradish peroxidase for the removal of p-chlorophenol from aqueous solution , 2005 .

[55]  C. Crestini,et al.  The early oxidative biodegradation steps of residual kraft lignin models with laccase. , 1998, Bioorganic & medicinal chemistry.

[56]  T. Tzanov,et al.  Decolorization and Detoxification of Textile Dyes with a Laccase from Trametes hirsuta , 2000, Applied and Environmental Microbiology.

[57]  C. Khosla,et al.  Modular enzymes : Biocatalysis: Synthesis methods that exploit enzymatic activities , 2001 .