TY - JOUR
T1 - Plasma-Driven in Situ Production of Hydrogen Peroxide for Biocatalysis
AU - Yayci, Abdulkadir
AU - Baraibar, Álvaro Gómez
AU - Krewing, Marco
AU - Fueyo, Elena Fernandez
AU - Hollmann, Frank
AU - Alcalde, Miguel
AU - Kourist, Robert
AU - Bandow, Julia E.
PY - 2020
Y1 - 2020
N2 - Peroxidases and peroxygenases are promising classes of enzymes for biocatalysis because of their ability to carry out one-electron oxidation reactions and stereoselective oxyfunctionalizations. However, industrial application is limited, as the major drawback is the sensitivity toward the required peroxide substrates. Herein, we report a novel biocatalysis approach to circumvent this shortcoming: in situ production of H2O2 by dielectric barrier discharge plasma. The discharge plasma can be controlled to produce hydrogen peroxide at desired rates, yielding desired concentrations. Using horseradish peroxidase, it is demonstrated that hydrogen peroxide produced by plasma treatment can drive the enzymatic oxidation of model substrates. Fungal peroxygenase is then employed to convert ethylbenzene to (R)-1-phenylethanol with an ee of >96 % using plasma-generated hydrogen peroxide. As direct treatment of the reaction solution with plasma results in reduced enzyme activity, the use of plasma-treated liquid and protection strategies are investigated to increase total turnover. Technical plasmas present a noninvasive means to drive peroxide-based biotransformations.
AB - Peroxidases and peroxygenases are promising classes of enzymes for biocatalysis because of their ability to carry out one-electron oxidation reactions and stereoselective oxyfunctionalizations. However, industrial application is limited, as the major drawback is the sensitivity toward the required peroxide substrates. Herein, we report a novel biocatalysis approach to circumvent this shortcoming: in situ production of H2O2 by dielectric barrier discharge plasma. The discharge plasma can be controlled to produce hydrogen peroxide at desired rates, yielding desired concentrations. Using horseradish peroxidase, it is demonstrated that hydrogen peroxide produced by plasma treatment can drive the enzymatic oxidation of model substrates. Fungal peroxygenase is then employed to convert ethylbenzene to (R)-1-phenylethanol with an ee of >96 % using plasma-generated hydrogen peroxide. As direct treatment of the reaction solution with plasma results in reduced enzyme activity, the use of plasma-treated liquid and protection strategies are investigated to increase total turnover. Technical plasmas present a noninvasive means to drive peroxide-based biotransformations.
KW - biocatalysis
KW - peroxidase
KW - peroxides
KW - peroxygenase
KW - plasma chemistry
UR - http://www.scopus.com/inward/record.url?scp=85081972917&partnerID=8YFLogxK
U2 - 10.1002/cssc.201903438
DO - 10.1002/cssc.201903438
M3 - Article
AN - SCOPUS:85081972917
SN - 1864-5631
VL - 13
SP - 2072
EP - 2079
JO - ChemSusChem
JF - ChemSusChem
IS - 8
ER -