Industrial Applications of Enzymes: Recent Advances, Techniques, and Outlooks

Enzymes as industrial biocatalysts offer numerous advantages over traditional chemical processes with respect to sustainability and process efficiency. Enzyme catalysis has been scaled up for commercial processes in the pharmaceutical, food and beverage industries, although further enhancements in stability and biocatalyst functionality are required for optimal biocatalytic processes in the energy sector for biofuel production and in natural gas conversion. The technical barriers associated with the implementation of immobilized enzymes suggest that a multidisciplinary approach is necessary for the development of immobilized biocatalysts applicable in such industrial-scale processes. Specifically, the overlap of technical expertise in enzyme immobilization, protein and process engineering will define the next generation of immobilized biocatalysts and the successful scale-up of their induced processes. This review discusses how biocatalysis has been successfully deployed, how enzyme immobilization can improve industrial processes, as well as focuses on the analysis tools critical for the multi-scale implementation of enzyme immobilization for increased product yield at maximum market profitability and minimum logistical burden on the environment and user.

[1]  P. Börjesson,et al.  Integrating enzyme fermentation in lignocellulosic ethanol production: life-cycle assessment and techno-economic analysis , 2017, Biotechnology for Biofuels.

[2]  Jung-Min Choi,et al.  Industrial applications of enzyme biocatalysis: Current status and future aspects. , 2015, Biotechnology advances.

[3]  Jo‐Shu Chang,et al.  Immobilization of Burkholderia sp. lipase on a ferric silica nanocomposite for biodiesel production. , 2012, Journal of biotechnology.

[4]  C. Cusan,et al.  Enzymatic synthesis of activated esters and their subsequent use in enzyme-based peptide synthesis , 2011 .

[5]  J. Thirkettle SB-253514 and analogues; novel inhibitors of lipoprotein associated phospholipase A2 produced by Pseudomonas fluorescens DSM 11579. III. Biotransformation using naringinase. , 2000, The Journal of antibiotics.

[6]  H. von Blottnitz,et al.  A life-cycle comparison between inorganic and biological catalysis for the production of biodiesel , 2008 .

[7]  M. Bhat,et al.  Cellulases and related enzymes in biotechnology. , 2000, Biotechnology advances.

[8]  Paul N. Devine,et al.  Biocatalytic Asymmetric Synthesis of Chiral Amines from Ketones Applied to Sitagliptin Manufacture , 2010, Science.

[9]  Vincenza Calabrò,et al.  Endo‐ and exo‐inulinases: Enzyme‐substrate interaction and rational immobilization , 2009, Biotechnology progress.

[10]  Olga Abian,et al.  Determination of protein‐protein interactions through aldehyde‐dextran intermolecular cross‐linking , 2004, Proteomics.

[11]  Pedro Fernandes,et al.  Enzymes in Food Processing: A Condensed Overview on Strategies for Better Biocatalysts , 2010, Enzyme research.

[12]  L. Gonçalves,et al.  Enzyme immobilization onto renewable polymeric matrixes: Past, present, and future trends , 2015 .

[13]  Jack Liang,et al.  Efficient, chemoenzymatic process for manufacture of the Boceprevir bicyclic [3.1.0]proline intermediate based on amine oxidase-catalyzed desymmetrization. , 2012, Journal of the American Chemical Society.

[14]  C. Fontes-Ribeiro,et al.  The dipeptidyl peptidase-4 (DPP-4) inhibitor sitagliptin ameliorates retinal endothelial cell dysfunction triggered by inflammation. , 2018, Biomedicine & pharmacotherapy = Biomedecine & pharmacotherapie.

[15]  Sushil Nagar,et al.  Covalent immobilization of organic solvent tolerant lipase on aluminum oxide pellets and its potential application in esterification reaction , 2013 .

[16]  B. Bhanage,et al.  Kinetic resolution of 1,2-diols using immobilized Burkholderia cepacia lipase: A combined experimental and molecular dynamics investigation. , 2017, Journal of biotechnology.

[17]  Roger A. Sheldon,et al.  Catalytic performance of cross-linked enzyme aggregates of Penicillium expansum lipase and their use as catalyst for biodiesel production , 2012 .

[18]  Shu-Wei Chang,et al.  Biocatalysis for the production of industrial products and functional foods from rice and other agricultural produce. , 2008, Journal of agricultural and food chemistry.

[19]  A. A. U. Souza,et al.  Cellulase immobilization on magnetic nanoparticles encapsulated in polymer nanospheres , 2017, Bioprocess and Biosystems Engineering.

[20]  P. N. Sarma,et al.  Nickel-Impregnated Silica Nanoparticle Synthesis and Their Evaluation for Biocatalyst Immobilization , 2010, Applied biochemistry and biotechnology.

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

[22]  R. Fernández-Lafuente,et al.  Stabilization of different alcohol oxidases via immobilization and post immobilization techniques , 2007 .

[23]  Wen Tong Chong,et al.  A review on potential enzymatic reaction for biofuel production from algae , 2014 .

[24]  Huimin Zhao,et al.  Biocatalysis for the synthesis of pharmaceuticals and pharmaceutical intermediates. , 2017, Bioorganic & medicinal chemistry.

[25]  C. Harms,et al.  Metolachlor, S-metolachlor and their role within sustainable weed-management , 1998 .

[26]  Ki‐Hyun Kim,et al.  Recent advances in enzyme immobilization techniques: Metal-organic frameworks as novel substrates , 2016 .

[27]  Aman A Desai,et al.  Sitagliptin manufacture: a compelling tale of green chemistry, process intensification, and industrial asymmetric catalysis. , 2011, Angewandte Chemie.

[28]  G. Chauhan Evaluation of nanogels as supports for enzyme immobilization , 2014 .

[29]  M. Zong,et al.  Recent advances in immobilized enzymes on nanocarriers , 2016 .

[30]  Roger M. Howard,et al.  Commercial Synthesis of (S,S)-Reboxetine Succinate: A Journey To Find the Cheapest Commercial Chemistry for Manufacture , 2011 .

[31]  Jianxin Jiang,et al.  Recent developments in activities, utilization and sources of cellulase , 2009 .

[32]  Fei Jia,et al.  Resolution of N-(2-ethyl-6-methylphenyl) alanine via cross-linked aggregates of Pseudomonas sp. Lipase , 2008 .

[33]  B. Shamasundar,et al.  Effect of oven drying and freeze drying on the antioxidant and functional properties of protein hydrolysates derived from freshwater fish (Cirrhinus mrigala) using papain enzyme , 2016, Journal of Food Science and Technology.

[34]  M. Y. Arica,et al.  Immobilization of catalase in poly(isopropylacrylamide‐co‐hydroxyethylmethacrylate) thermally reversible hydrogels , 1999 .

[35]  D. Freire,et al.  Nanomaterials for biocatalyst immobilization – state of the art and future trends , 2016 .

[36]  H. F. de Castro,et al.  Immobilization of a Commercial Lipase from Penicillium camembertii (Lipase G) by Different Strategies , 2011, Enzyme research.

[37]  L. Betancor,et al.  Bioinspired enzyme encapsulation for biocatalysis. , 2008, Trends in biotechnology.

[38]  R. Sheldon,et al.  Cross-linked enzyme aggregates: a simple and effective method for the immobilization of penicillin acylase. , 2000, Organic letters.

[39]  Chengdong Zhang,et al.  Activity of catalase adsorbed to carbon nanotubes: effects of carbon nanotube surface properties. , 2013, Talanta.

[40]  Lubbert Dijkhuizen,et al.  Properties and applications of starch-converting enzymes of the α-amylase family , 2002 .

[41]  Azmi Telefoncu,et al.  Improving the stability of cellulase by immobilization on modified polyvinyl alcohol coated chitosan beads , 2007 .

[42]  Hongjuan Ma,et al.  Covalent-bonded immobilization of enzyme on hydrophilic polymer covering magnetic nanogels , 2008 .

[43]  Gareth R. Williams,et al.  Electrospun polyacrylonitrile-glycopolymer nanofibrous membranes for enzyme immobilization , 2012 .

[44]  Krist V. Gernaey,et al.  Advances in the Process Development of Biocatalytic Processes , 2013 .

[45]  J. Ge,et al.  Facile synthesis of multiple enzyme-containing metal-organic frameworks in a biomolecule-friendly environment. , 2015, Chemical communications.

[46]  M. Taherzadeh,et al.  Enzyme-based hydrolysis processes for ethanol from lignocellulosic materials: A review , 2007, BioResources.

[47]  A. Grigoras Catalase immobilization—A review , 2017 .

[48]  Kun-Lin Yang,et al.  Combined cross-linked enzyme aggregates of horseradish peroxidase and glucose oxidase for catalyzing cascade chemical reactions. , 2017, Enzyme and microbial technology.

[49]  N. Weber,et al.  Preparation of lipophilic alkyl (hydroxy)benzoates by solvent-free lipase-catalyzed esterification and transesterification , 2008, Applied Microbiology and Biotechnology.

[50]  Abdul Hameed,et al.  Industrial applications of microbial lipases , 2006 .

[51]  P. Strong,et al.  Methane as a resource: can the methanotrophs add value? , 2015, Environmental science & technology.

[52]  K. Khorshidi,et al.  Preparation and characterization of nanomagnetic cross-linked cellulase aggregates for cellulose bioconversion , 2016 .

[53]  J. Cui,et al.  Cross-Linked Enzyme Aggregates of Phenylalanine Ammonia Lyase: Novel Biocatalysts for Synthesis of L-Phenylalanine , 2012, Applied Biochemistry and Biotechnology.

[54]  Q. Fei,et al.  Bioconversion of natural gas to liquid fuel: opportunities and challenges. , 2014, Biotechnology advances.

[55]  H. Treichel,et al.  Application of home-made lipase in the production of geranyl propionate by esterification of geraniol and propionic acid in solvent-free system , 2015 .

[56]  M. Nunes,et al.  Exploring magnetic and imprinted cross-linked enzyme aggregates of rhamnopyranosidase in microbioreactors. , 2018, Bioresource technology.

[57]  M. Alfa,et al.  A new hydrogen peroxide--based medical-device detergent with germicidal properties: comparison with enzymatic cleaners. , 2001, American journal of infection control.

[58]  Bernd Nidetzky,et al.  Positively charged mini-protein Zbasic2 as a highly efficient silica binding module: opportunities for enzyme immobilization on unmodified silica supports. , 2012, Langmuir : the ACS journal of surfaces and colloids.

[59]  Brooks D. Rabideau,et al.  Mechanisms of hydrogen bond formation between ionic liquids and cellulose and the influence of water content. , 2015, Physical chemistry chemical physics : PCCP.

[60]  Diannan Lu,et al.  Fabrication of single carbonic anhydrase nanogel against denaturation and aggregation at high temperature. , 2007, Biomacromolecules.

[61]  T. Tan,et al.  Biodiesel production with immobilized lipase: A review. , 2010, Biotechnology advances.

[62]  Richard A. Cunha,et al.  Designing an enzyme-based nanobiosensor using molecular modeling techniques. , 2011, Physical chemistry chemical physics : PCCP.

[63]  J. Mcauliffe,et al.  Industrial use of immobilized enzymes. , 2013, Chemical Society reviews.

[64]  B. Bhanage,et al.  Enhanced biocatalytic activity of immobilized Pseudomonas cepacia lipase under sonicated condition , 2016, Bioprocess and Biosystems Engineering.

[65]  Dehua Liu,et al.  Lipase-catalyzed process for biodiesel production: Enzyme immobilization, process simulation and optimization , 2015 .

[66]  P. Christakopoulos,et al.  Preparation of multipurpose cross-linked enzyme aggregates and their application to production of alkyl ferulates , 2008 .

[67]  R. Sheldon Cross-Linked Enzyme Aggregates as Industrial Biocatalysts , 2011 .

[68]  P. Bajpai Application of Enzymes in the Pulp and Paper Industry , 1999, Biotechnology progress.

[69]  Yung-Chuan Liu,et al.  Kinetics and optimization of lipase-catalyzed synthesis of rose fragrance 2-phenylethyl acetate through transesterification , 2014 .

[70]  Junhua Tao,et al.  Development of a Chemoenzymatic Manufacturing Process for Pregabalin , 2008 .

[71]  John M. Woodley,et al.  Role of Biocatalysis in Sustainable Chemistry. , 2017, Chemical reviews.

[72]  Manoj Kumar,et al.  Microbial enzymes: industrial progress in 21st century , 2016, 3 Biotech.

[73]  J. Fernández‐Lucas,et al.  New trends for a classical enzyme: Papain, a biotechnological success story in the food industry , 2017 .

[74]  Ramesh N. Patel,et al.  Biocatalysis for synthesis of pharmaceuticals. , 2017, Bioorganic & medicinal chemistry.

[75]  Rishi Gupta,et al.  Microbial Cellulases and Their Industrial Applications , 2011, Enzyme research.

[76]  Ipsita Roy,et al.  Converting Enzymes into Tools of Industrial Importance. , 2017, Recent patents on biotechnology.

[77]  A. Petri,et al.  Efficient immobilization of epoxide hydrolase onto silica gel and use in the enantioselective hydrolysis of racemic para-nitrostyrene oxide , 2005 .

[78]  M. Danquah,et al.  Industrial-scale manufacturing of pharmaceutical-grade bioactive peptides. , 2011, Biotechnology advances.

[79]  B. Krajewska,et al.  Enzyme immobilization by adsorption: a review , 2014, Adsorption.

[80]  Guonan Chen,et al.  Facile synthesis of enzyme–inorganic hybrid nanoflowers and their application as an immobilized trypsin reactor for highly efficient protein digestion , 2014 .

[81]  M. Mazutti,et al.  Effect of Organic Solvent on the Characteristics of Free and Immobilized Inulinase from Kluyveromyces marxianus ATCC 16045 , 2010 .

[82]  S. Ansari,et al.  Potential applications of enzymes immobilized on/in nano materials: A review. , 2012, Biotechnology advances.

[83]  Edgar Voss,et al.  Enzyme-catalyzed processes in pharmaceutical industry , 2001 .

[84]  Shusheng Pang,et al.  Ionic liquids and their interaction with cellulose. , 2009, Chemical reviews.

[85]  D. Oliveira,et al.  A review on enzymatic synthesis of aromatic esters used as flavor ingredients for food, cosmetics and pharmaceuticals industries , 2017 .

[86]  Radivoje Prodanovic,et al.  Immobilization of lipase from Candida rugosa on Eupergit® C supports by covalent attachment , 2006 .

[87]  J. V. Edwards,et al.  Immobilization of lysozyme-cellulose amide-linked conjugates on cellulose I and II cotton nanocrystalline preparations , 2012, Cellulose.

[88]  Diána Weiser,et al.  A Continuous‐Flow Cascade Reactor System for Subtilisin A‐ Catalyzed Dynamic Kinetic Resolution of N‐tert‐Butyloxycarbonylphenylalanine Ethyl Thioester with Benzylamine , 2016 .

[89]  R. Sheldon Characteristic features and biotechnological applications of cross-linked enzyme aggregates (CLEAs) , 2011, Applied Microbiology and Biotechnology.

[90]  R. Stevanato,et al.  Cysteine enhances activity and stability of immobilized papain , 2010, Amino Acids.

[91]  Frances H Arnold,et al.  Directed enzyme evolution: climbing fitness peaks one amino acid at a time. , 2009, Current opinion in chemical biology.

[92]  Prerana D. Tomke,et al.  Ultrasound assisted lipase catalyzed synthesis of cinnamyl acetate via transesterification reaction in a solvent free medium. , 2015, Ultrasonics sonochemistry.

[93]  N. Gupta,et al.  Hollow Silica Nanoparticles as Support for Catalase Enzyme Immobilization , 2013, Catalysis Letters.

[94]  Lutz Hilterhaus,et al.  Evaluation of immobilized enzymes for industrial applications. , 2013, Chemical Society reviews.

[95]  Alan S. Campbell,et al.  Perhydrolase-nanotube-paint sporicidal composites stabilized by intramolecular crosslinking , 2012 .

[96]  Fa-An Chao,et al.  Structure and dynamics of a primordial catalytic fold generated by in vitro evolution , 2012, Nature chemical biology.

[97]  C. Bernal,et al.  BIOTECHNOLOGICALLY RELEVANT ENZYMES AND PROTEINS Enhanced long-chain fatty alcohol oxidation by immobilization of alcohol dehydrogenase from S . cerevisiae , 2017 .

[98]  Alessandro Pellis,et al.  Evolving biocatalysis to meet bioeconomy challenges and opportunities. , 2018, New biotechnology.

[99]  Kyle A. Stone,et al.  A mini review on bioreactor configurations and gas transfer enhancements for biochemical methane conversion , 2017 .

[100]  Shuang Li,et al.  Technology Prospecting on Enzymes: Application, Marketing and Engineering , 2012, Computational and structural biotechnology journal.

[101]  Mohammad J. Taherzadeh,et al.  ENZYMATIC-BASED HYDROLYSIS PROCESSES FOR ETHANOL , 2007 .

[102]  Changyou Gao,et al.  Immobilization of enzymes on 2-hydroxyethyl methacrylate and glycidyl methacrylate copolymer brushes. , 2014, Chemistry, an Asian journal.

[103]  Hesham M. Marouf Effect of Pregabalin Premedication on Emergence Agitation in Children after Sevoflurane Anesthesia: A Randomized Controlled Study , 2018, Anesthesia, essays and researches.

[104]  L. Makowski,et al.  Multi-scale processes of beech wood disintegration and pretreatment with 1-ethyl-3-methylimidazolium acetate/water mixtures , 2016, Biotechnology for Biofuels.

[105]  S. Krishnan,et al.  Stability, Scalability, and Reusability of a Volume Efficient Biocatalytic System Constructed on Magnetic Nanoparticles. , 2016, Catalysis science & technology.

[106]  Yun Lin,et al.  A simple and convenient method for the preparation of antioxidant peptides from walnut (Juglans regia L.) protein hydrolysates , 2016, Chemistry Central Journal.

[107]  Shweta Kumari,et al.  Biotechnological approaches for the production of prebiotics and their potential applications , 2013, Critical reviews in biotechnology.

[108]  C. Cardona,et al.  Production of bioethanol from sugarcane bagasse: Status and perspectives. , 2010, Bioresource technology.

[109]  A. Illanes,et al.  Production of cephalexin in organic medium at high substrate concentrations with CLEA of penicillin acylase and PGA-450 , 2007 .

[110]  Sarah E. Baker,et al.  Printable enzyme-embedded materials for methane to methanol conversion , 2016, Nature Communications.

[111]  M. Wetzstein,et al.  Considering macroeconomic indicators in the food before fuel nexus , 2012 .

[112]  A. Leuchter,et al.  Evaluation of reboxetine, a noradrenergic antidepressant, for the treatment of fibromyalgia and chronic low back pain. , 2005, Psychosomatics.

[113]  R. Bruckner,et al.  Probing oxygen activation sites in two flavoprotein oxidases using chloride as an oxygen surrogate. , 2011, Biochemistry.

[114]  Ravindra Pogaku,et al.  Life cycle assessment of biodiesel production using alkali, soluble and immobilized enzyme catalyst processes , 2011 .

[115]  Rachna Verma,et al.  Microbial Proteases and Application as Laundry Detergent Additive , 2008 .

[116]  Gang Sun,et al.  Lipase immobilization on glutaraldehyde-activated nanofibrous membranes for improved enzyme stabilities and activities , 2012 .

[117]  Rolf Dach,et al.  The Eight Criteria Defining a Good Chemical Manufacturing Process , 2012 .

[118]  W P Clarke,et al.  A methanotroph-based biorefinery: Potential scenarios for generating multiple products from a single fermentation. , 2016, Bioresource technology.

[119]  J. Woodley,et al.  Application of environmental and economic metrics to guide the development of biocatalytic processes , 2014 .

[120]  J. Lennerstrand,et al.  The effect of the first-generation HCV-protease inhibitors boceprevir and telaprevir and the relation to baseline NS3 resistance mutations in genotype 1: experience from a small Swedish cohort , 2018, Upsala journal of medical sciences.

[121]  Aasima Rafiq,et al.  Protein engineering and its applications in food industry , 2017, Critical reviews in food science and nutrition.

[122]  Hafiz M.N. Iqbal,et al.  Recent trends and valorization of immobilization strategies and ligninolytic enzymes by industrial biotechnology , 2014 .

[123]  Bernd Nidetzky,et al.  Smart enzyme immobilization in microstructured reactors , 2013 .

[124]  Bo Jin,et al.  Nanobiocatalyst advancements and bioprocessing applications , 2015, Journal of The Royal Society Interface.

[125]  Andreas S Bommarius,et al.  Stabilizing biocatalysts. , 2013, Chemical Society reviews.

[126]  Peijun Ji,et al.  Enzymes immobilized on carbon nanotubes. , 2011, Biotechnology advances.

[127]  H. Leemhuis,et al.  Properties and applications of starch-converting enzymes of the alpha-amylase family. , 2002, Journal of biotechnology.

[128]  Gjalt W Huisman,et al.  On the development of new biocatalytic processes for practical pharmaceutical synthesis. , 2013, Current opinion in chemical biology.

[129]  Hao Zhou,et al.  Catalytic performance and molecular dynamic simulation of immobilized CC bond hydrolase based on carbon nanotube matrix. , 2014, Colloids and surfaces. B, Biointerfaces.

[130]  Parameswaran Binod,et al.  Strategies for design of improved biocatalysts for industrial applications. , 2017, Bioresource technology.

[131]  G. Feijoo,et al.  Combined cross-linked enzyme aggregates from versatile peroxidase and glucose oxidase: production, partial characterization and application for the elimination of endocrine disruptors. , 2011, Bioresource technology.

[132]  Denny K. S. Ng,et al.  Review of evolution, technology and sustainability assessments of biofuel production , 2014 .

[133]  B. Zhang,et al.  Enzyme immobilization for biodiesel production , 2011, Applied Microbiology and Biotechnology.

[134]  D. Yıldırım,et al.  Immobilization of catalase onto Eupergit C and its characterization , 2010 .

[135]  M. L. Ferreira,et al.  Immobilization of catalase from Aspergillus niger on inorganic and biopolymeric supports for H2O2 decomposition , 2004 .