TY - JOUR
T1 - Nuclear Waste and Biocatalysis
T2 - A Sustainable Liaison?
AU - Zhang, Wuyuan
AU - Liu, Huanhuan
AU - Van Schie, Morten M.C.H.
AU - Hagedoorn, Peter Leon
AU - Alcalde, Miguel
AU - Denkova, Antonia G.
AU - Djanashvili, Kristina
AU - Hollmann, Frank
PY - 2020
Y1 - 2020
N2 - It is well-known that energy-rich radiation induces water splitting, eventually yielding hydrogen peroxide. Synthetic applications, however, are scarce and to the best of our knowledge, the combination of radioactivity with enzyme-catalysis has not been considered yet. Peroxygenases utilize H2O2 as an oxidant to promote highly selective oxyfunctionalization reactions but are also irreversibly inactivated in the presence of too high H2O2 concentrations. Therefore, there is a need for efficient in situ H2O2 generation methods. Here, we show that radiolytic water splitting can be used to promote specific biocatalytic oxyfunctionalization reactions. Parameters influencing the efficiency of the reaction and current limitations are shown. Particularly, oxidative inactivation of the biocatalyst by hydroxyl radicals influences the robustness of the overall reaction. Radical scavengers can alleviate this issue, but eventually, physical separation of the enzymes from the ionizing radiation will be necessary to achieve robust reaction schemes. We demonstrate that nuclear waste can also be used to drive selective, peroxygenase-catalyzed oxyfunctionalization reactions, challenging our view on nuclear waste in terms of sustainability.
AB - It is well-known that energy-rich radiation induces water splitting, eventually yielding hydrogen peroxide. Synthetic applications, however, are scarce and to the best of our knowledge, the combination of radioactivity with enzyme-catalysis has not been considered yet. Peroxygenases utilize H2O2 as an oxidant to promote highly selective oxyfunctionalization reactions but are also irreversibly inactivated in the presence of too high H2O2 concentrations. Therefore, there is a need for efficient in situ H2O2 generation methods. Here, we show that radiolytic water splitting can be used to promote specific biocatalytic oxyfunctionalization reactions. Parameters influencing the efficiency of the reaction and current limitations are shown. Particularly, oxidative inactivation of the biocatalyst by hydroxyl radicals influences the robustness of the overall reaction. Radical scavengers can alleviate this issue, but eventually, physical separation of the enzymes from the ionizing radiation will be necessary to achieve robust reaction schemes. We demonstrate that nuclear waste can also be used to drive selective, peroxygenase-catalyzed oxyfunctionalization reactions, challenging our view on nuclear waste in terms of sustainability.
KW - biocatalysis
KW - oxyfunctionalization
KW - peroxygenases
KW - radiation
KW - sustainability
UR - http://www.scopus.com/inward/record.url?scp=85097797952&partnerID=8YFLogxK
U2 - 10.1021/acscatal.0c03059
DO - 10.1021/acscatal.0c03059
M3 - Article
AN - SCOPUS:85097797952
SN - 2155-5435
VL - 10
SP - 14195
EP - 14200
JO - ACS Catalysis
JF - ACS Catalysis
IS - 23
ER -