Advancing Biocatalysis through Enzyme, Cellular, and Platform Engineering

Biocatalysis offers opportunities for highly selective chemical reactions with high turnover rates under relatively mild conditions. Use of whole‐cell or multi‐enzyme systems enables transformations of complexity unmatched by nonbiological routes. However, advantages of biocatalysis are frequently compromised by poor enzymatic performance under non‐native reaction conditions, the absence of enzymes with desired substrate or reaction specificities, and low metabolic fluxes or competing pathways. During the 234th National Meeting of the American Chemical Society, these issues were addressed in the “Advances in Biocatalysis” sessions. Protein engineering and metabolic pathway engineering were used to develop efficient enzymes and whole‐cell catalysts. Novel strategies for the use of enzymes at solid interfaces and in nonaqueous environments were discussed, and efficient biotransformation platforms were demonstrated. These advances broaden the applications of biocatalysis in biofuels, pharmaceuticals, fine chemicals, and human health.

[1]  J. Stein,et al.  Biological activities of resveratrol and its analogs , 2002 .

[2]  C. Schmidt-Dannert,et al.  Biosynthesis of plant-specific stilbene polyketides in metabolically engineered Escherichia coli , 2006, BMC biotechnology.

[3]  Moo-Yeal Lee,et al.  Metabolizing enzyme toxicology assay chip (MetaChip) for high-throughput microscale toxicity analyses. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[4]  J. Dordick,et al.  Enzyme activation for nonaqueous media. , 2002, Current opinion in biotechnology.

[5]  M. Koffas,et al.  Expression of a soluble flavone synthase allows the biosynthesis of phytoestrogen derivatives in Escherichia coli , 2006, Applied Microbiology and Biotechnology.

[6]  Huimin Zhao,et al.  Recent advances in biocatalysis by directed enzyme evolution. , 2006, Combinatorial chemistry & high throughput screening.

[7]  D. Demirjian,et al.  Screening for Novel Enzymes , 1999 .

[8]  Huimin Zhao,et al.  Heterologous Expression, Purification, and Characterization of a Highly Active Xylose Reductase from Neurospora crassa , 2005, Applied and Environmental Microbiology.

[9]  M. Koffas,et al.  Biosynthesis of Natural Flavanones in Saccharomyces cerevisiae , 2005, Applied and Environmental Microbiology.

[10]  K. Vorlop,et al.  Industrial bioconversion of renewable resources as an alternative to conventional chemistry , 2004, Applied Microbiology and Biotechnology.

[11]  Jennifer A. Prescher,et al.  Discovery of aminoacyl-tRNA synthetase activity through cell-surface display of noncanonical amino acids , 2006, Proceedings of the National Academy of Sciences.

[12]  Zhen Yang,et al.  Ionic liquids: Green solvents for nonaqueous biocatalysis , 2005 .

[13]  Lei Wang,et al.  Expanding the Genetic Code , 2003, Science.

[14]  Ravi S Kane,et al.  Increasing protein stability through control of the nanoscale environment. , 2006, Langmuir : the ACS journal of surfaces and colloids.

[15]  L. Ingram,et al.  Engineering Escherichia coli for xylitol production from glucose‐xylose mixtures , 2006, Biotechnology and bioengineering.

[16]  M. Koffas,et al.  Engineering Central Metabolic Pathways for High-Level Flavonoid Production in Escherichia coli , 2007, Applied and Environmental Microbiology.

[17]  Yi Tang,et al.  Efficient Synthesis of Simvastatin by Use of Whole-Cell Biocatalysis , 2007, Applied and Environmental Microbiology.

[18]  T. Yoo,et al.  Evolution of a fluorinated green fluorescent protein , 2007, Proceedings of the National Academy of Sciences.

[19]  Kenji Watanabe,et al.  Biosynthesis of lovastatin analogs with a broadly specific acyltransferase. , 2006, Chemistry & biology.

[20]  Frances H Arnold,et al.  Global incorporation of norleucine in place of methionine in cytochrome P450 BM‐3 heme domain increases peroxygenase activity , 2003, Biotechnology and bioengineering.

[21]  P. Kambam,et al.  Engineering and applications of genetic circuits. , 2007, Molecular bioSystems.

[22]  Y. Chuang,et al.  Fluorescent intensity of a novel NADPH-binding protein of Vibrio vulnificus can be improved by directed evolution. , 2004, Biochemical and biophysical research communications.

[23]  E. P. Hudson,et al.  Biocatalysis in semi-aqueous and nearly anhydrous conditions. , 2005, Current opinion in biotechnology.

[24]  G. Stephanopoulos,et al.  Global transcription machinery engineering: a new approach for improving cellular phenotype. , 2007, Metabolic engineering.

[25]  Y. Chuang,et al.  Cloning and characterization of a blue fluorescent protein from Vibrio vulnificus. , 2001, Biochemical and biophysical research communications.

[26]  Timothy A. Whitehead,et al.  A filamentous molecular chaperone of the prefoldin family from the deep‐sea hyperthermophile Methanocaldococcus jannaschii , 2007, Protein science : a publication of the Protein Society.

[27]  P. Kambam,et al.  Noise and kinetics of LuxR positive feedback loops. , 2007, Biochemical and biophysical research communications.

[28]  David A. Tirrell,et al.  Non‐Canonical Amino Acids in Protein Polymer Design , 2007 .

[29]  D. Clark,et al.  Water dynamics and salt-activation of enzymes in organic media: mechanistic implications revealed by NMR spectroscopy. , 2006, Proceedings of the National Academy of Sciences of the United States of America.

[30]  Huimin Zhao,et al.  Efficient regeneration of NADPH using an engineered phosphite dehydrogenase , 2007, Biotechnology and bioengineering.

[31]  Nikhil U. Nair,et al.  Biochemical Characterization of an l-Xylulose Reductase from Neurospora crassa , 2007, Applied and Environmental Microbiology.

[32]  R. Sheldon,et al.  Biocatalytic transformations in ionic liquids. , 2003, Trends in biotechnology.

[33]  Lishan Zhao,et al.  Bioethanol. , 2006, Current opinion in chemical biology.

[34]  W. Wong,et al.  Improving simvastatin bioconversion in Escherichia coli by deletion of bioH. , 2007, Metabolic engineering.

[35]  Johnathan E. Holladay,et al.  Top Value Added Chemicals From Biomass. Volume 1 - Results of Screening for Potential Candidates From Sugars and Synthesis Gas , 2004 .

[36]  Dietmar Haltrich,et al.  Continuous enzymatic regeneration of redox mediators used in biotransformation reactions employing flavoproteins , 2001 .

[37]  Daniel J. Sayut,et al.  Construction and engineering of positive feedback loops. , 2006, ACS chemical biology.

[38]  R. Kane,et al.  Water‐soluble carbon nanotube‐enzyme conjugates as functional biocatalytic formulations , 2006, Biotechnology and bioengineering.

[39]  G. Stephanopoulos,et al.  Engineering Yeast Transcription Machinery for Improved Ethanol Tolerance and Production , 2006, Science.

[40]  J. Dordick,et al.  High-throughput human metabolism and toxicity analysis. , 2006, Current opinion in biotechnology.

[41]  M A Henson,et al.  Design and mathematical modelling of a synthetic symbiotic ecosystem. , 2008, IET systems biology.

[42]  S. Resnick,et al.  Diverse reactions catalyzed by naphthalene dioxygenase fromPseudomonas sp strain NCIB 9816 , 1996, Journal of Industrial Microbiology.

[43]  Peter G. Schultz,et al.  A chemical toolkit for proteins — an expanded genetic code , 2006, Nature Reviews Molecular Cell Biology.

[44]  J. Pellegrino,et al.  Opportunities in the industrial biobased products industry , 2004, Applied biochemistry and biotechnology.

[45]  Keith E. J. Tyo,et al.  Expanding the metabolic engineering toolbox: more options to engineer cells. , 2007, Trends in biotechnology.

[46]  T. Yoo,et al.  High-throughput screening for methionyl-tRNA synthetases that enable residue-specific incorporation of noncanonical amino acids into recombinant proteins in bacterial cells. , 2007, Angewandte Chemie.

[47]  F. Arnold,et al.  Protein engineering of oxygenases for biocatalysis. , 2002, Current opinion in chemical biology.

[48]  J. T. Gerig,et al.  Motion at the active site of [(4-fluorophenyl)sulfonyl]chymotrypsin. , 1986, Biochemistry.

[49]  D. Haltrich,et al.  Continuous Enzymatic Regeneration of Electron Acceptors Used by Flavoenzymes: Cellobiose Dehydrogenase-Catalyzed Production of Lactobionic Acid as an Example , 2004 .

[50]  J. Stewart,et al.  Understanding and Improving NADPH‐Dependent Reactions by Nongrowing Escherichia coli Cells , 2008, Biotechnology progress.