Non-aqueous homogenous biocatalytic conversion of polysaccharides in ionic liquids using chemically modified glucosidase

被引:86
作者
Brogan, Alex P. S. [1 ]
Bui-Le, Liem [1 ]
Hallett, Jason P. [1 ]
机构
[1] Imperial Coll London, Dept Chem Engn, Exhibit Rd, London, England
基金
英国工程与自然科学研究理事会;
关键词
CIRCULAR-DICHROISM SPECTROSCOPY; SECONDARY STRUCTURE ANALYSES; ORGANIC-SOLVENTS; BIOMASS; ENZYMES; DECONSTRUCTION; NANOCONSTRUCTS; MYOGLOBIN; BIOFUELS; WATER;
D O I
10.1038/s41557-018-0088-6
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The increasing requirement to produce platform chemicals and fuels from renewable sources means advances in biocatalysis are rapidly becoming a necessity. Biomass is widely used in nature as a source of energy and as chemical building blocks. However, recalcitrance towards traditional chemical processes and solvents provides a significant barrier to widespread utility. Here, by optimizing enzyme solubility in ionic liquids, we have discovered solvent-induced substrate promiscuity of glucosidase, demonstrating an unprecedented example of homogeneous enzyme bioprocessing of cellulose. Specifically, chemical modification of glucosidase for solubilization in ionic liquids can increase thermal stability to up to 137 degrees C, allowing for enzymatic activity 30 times greater than is possible in aqueous media. These results establish that through a synergistic combination of chemical biology (enzyme modification) and reaction engineering (solvent choice), the biocatalytic capability of enzymes can be intensified: a key step towards the full-scale deployment of industrial biocatalysis.
引用
收藏
页码:859 / 865
页数:7
相关论文
共 30 条
  • [1] Understanding the polarity of ionic liquids
    Ab Rani, M. A.
    Brant, A.
    Crowhurst, L.
    Dolan, A.
    Lui, M.
    Hassan, N. H.
    Hallett, J. P.
    Hunt, P. A.
    Niedermeyer, H.
    Perez-Arlandis, J. M.
    Schrems, M.
    Welton, T.
    Wilding, R.
    [J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (37) : 16831 - 16840
  • [2] Biomass deconstruction to sugars
    Blanch, Harvey W.
    Simmons, Blake A.
    Klein-Marcuschamer, Daniel
    [J]. BIOTECHNOLOGY JOURNAL, 2011, 6 (09) : 1086 - 1102
  • [3] Deconstruction of lignocellulosic biomass with ionic liquids
    Brandt, Agnieszka
    Grasvik, John
    Hallett, Jason P.
    Welton, Tom
    [J]. GREEN CHEMISTRY, 2013, 15 (03) : 550 - 583
  • [4] Molecular Dynamics Simulations Reveal a Dielectric-Responsive Coronal Structure in Protein-Polymer Surfactant Hybrid Nanoconstructs
    Brogan, Alex P. S.
    Sessions, Richard B.
    Perriman, Adam W.
    Mann, Stephen
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (48) : 16824 - 16831
  • [5] Enzyme activity in liquid lipase melts as a step towards solvent-free biology at 150 °C
    Brogan, Alex P. S.
    Sharma, Kamendra P.
    Perriman, Adam W.
    Mann, Stephen
    [J]. NATURE COMMUNICATIONS, 2014, 5
  • [6] Hyper-thermal stability and unprecedented re-folding of solvent-free liquid myoglobin
    Brogan, Alex P. S.
    Siligardi, Giuliano
    Hussain, Rohanah
    Perriman, Adam W.
    Mann, Stephen
    [J]. CHEMICAL SCIENCE, 2012, 3 (06) : 1839 - 1846
  • [7] Solubilizing and Stabilizing Proteins in Anhydrous Ionic Liquids through Formation of Protein-Polymer Surfactant Nanoconstructs
    Brogans, Alex P. S.
    Halleet, Jason P.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (13) : 4494 - 4501
  • [8] Characteristics of nearly dry enzymes in organic solvents: implications for biocatalysis in the absence of water
    Clark, DS
    [J]. PHILOSOPHICAL TRANSACTIONS OF THE ROYAL SOCIETY OF LONDON SERIES B-BIOLOGICAL SCIENCES, 2004, 359 (1448) : 1299 - 1307
  • [9] A Polymer Surfactant Corona Dynamically Replaces Water in Solvent-Free Protein Liquids and Ensures Macromolecular Flexibility and Activity
    Gallat, Francois-Xavier
    Brogan, Alex P. S.
    Fichou, Yann
    McGrath, Nina
    Moulin, Martine
    Haertlein, Michael
    Combet, Jerome
    Wuttke, Joachim
    Mann, Stephen
    Zaccai, Giuseppe
    Jackson, Colin J.
    Perriman, Adam W.
    Weik, Martin
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (32) : 13168 - 13171
  • [10] George A, 2015, GREEN CHEM, V17, P1728, DOI [10.1039/C4GC01208A, 10.1039/c4gc01208a]