Cascading g-C3N4 and Peroxygenases for Selective Oxyfunctionalization Reactions

Morten M.C.H. Van Schie; Wuyuan Zhang; Florian Tieves; Da Som Choi; Chan Beum Park; Bastien O. Burek; Jonathan Z. Bloh; Isabel W.C.E. Arends; Caroline E. Paul; Miguel Alcalde; Frank Hollmann

doi:10.1021/acscatal.9b01341

Cascading g-C₃N₄ and Peroxygenases for Selective Oxyfunctionalization Reactions

Morten M.C.H. Van Schie^*, Wuyuan Zhang, Florian Tieves, Da Som Choi, Chan Beum Park, Bastien O. Burek, Jonathan Z. Bloh, Isabel W.C.E. Arends, Caroline E. Paul, Miguel Alcalde, Frank Hollmann

^*Corresponding author for this work

BT/Biocatalysis

Research output: Contribution to journal › Article › Scientific › peer-review

61 Citations (Scopus)

102 Downloads (Pure)

Abstract

Peroxygenases are very interesting catalysts for specific oxyfunctionalization chemistry. Instead of relying on complicated electron transport chains, they rely on simple hydrogen peroxide as the stoichiometric oxidant. Their poor robustness against H₂O₂ can be addressed via in situ generation of H₂O₂. Here we report that simple graphitic carbon nitride (g-C₃N₄) is a promising photocatalyst to drive peroxygenase-catalyzed hydroxylation reactions. The system has been characterized by outlining not only its scope but also its current limitations. In particular, spatial separation of the photocatalyst from the enzyme is shown as a solution to circumvent the undesired inactivation of the biocatalyst. Overall, very promising turnover numbers of the biocatalyst of more than 60.000 have been achieved.

Original language	English
Pages (from-to)	7409-7417
Journal	ACS Catalysis
Volume	9
Issue number	8
DOIs	https://doi.org/10.1021/acscatal.9b01341
Publication status	Published - 2019

Keywords

cascade reactions
enzyme catalysis
oxidation
oxyfunctionalization
photocatalysis

Access to Document

10.1021/acscatal.9b01341

acscatal.9b01341Final published version, 2.02 MBLicence: CC BY-NC-ND

Cite this

@article{43e3eb49af3b4287aa2b5497e0d7f00a,

title = "Cascading g-C3N4 and Peroxygenases for Selective Oxyfunctionalization Reactions",

abstract = "Peroxygenases are very interesting catalysts for specific oxyfunctionalization chemistry. Instead of relying on complicated electron transport chains, they rely on simple hydrogen peroxide as the stoichiometric oxidant. Their poor robustness against H2O2 can be addressed via in situ generation of H2O2. Here we report that simple graphitic carbon nitride (g-C3N4) is a promising photocatalyst to drive peroxygenase-catalyzed hydroxylation reactions. The system has been characterized by outlining not only its scope but also its current limitations. In particular, spatial separation of the photocatalyst from the enzyme is shown as a solution to circumvent the undesired inactivation of the biocatalyst. Overall, very promising turnover numbers of the biocatalyst of more than 60.000 have been achieved.",

keywords = "cascade reactions, enzyme catalysis, oxidation, oxyfunctionalization, photocatalysis",

author = "{Van Schie}, {Morten M.C.H.} and Wuyuan Zhang and Florian Tieves and Choi, {Da Som} and Park, {Chan Beum} and Burek, {Bastien O.} and Bloh, {Jonathan Z.} and Arends, {Isabel W.C.E.} and Paul, {Caroline E.} and Miguel Alcalde and Frank Hollmann",

year = "2019",

doi = "10.1021/acscatal.9b01341",

language = "English",

volume = "9",

pages = "7409--7417",

journal = "ACS Catalysis",

issn = "2155-5435",

publisher = "American Chemical Society (ACS)",

number = "8",

}

TY - JOUR

T1 - Cascading g-C3N4 and Peroxygenases for Selective Oxyfunctionalization Reactions

AU - Van Schie, Morten M.C.H.

AU - Zhang, Wuyuan

AU - Tieves, Florian

AU - Choi, Da Som

AU - Park, Chan Beum

AU - Burek, Bastien O.

AU - Bloh, Jonathan Z.

AU - Arends, Isabel W.C.E.

AU - Paul, Caroline E.

AU - Alcalde, Miguel

AU - Hollmann, Frank

PY - 2019

Y1 - 2019

N2 - Peroxygenases are very interesting catalysts for specific oxyfunctionalization chemistry. Instead of relying on complicated electron transport chains, they rely on simple hydrogen peroxide as the stoichiometric oxidant. Their poor robustness against H2O2 can be addressed via in situ generation of H2O2. Here we report that simple graphitic carbon nitride (g-C3N4) is a promising photocatalyst to drive peroxygenase-catalyzed hydroxylation reactions. The system has been characterized by outlining not only its scope but also its current limitations. In particular, spatial separation of the photocatalyst from the enzyme is shown as a solution to circumvent the undesired inactivation of the biocatalyst. Overall, very promising turnover numbers of the biocatalyst of more than 60.000 have been achieved.

AB - Peroxygenases are very interesting catalysts for specific oxyfunctionalization chemistry. Instead of relying on complicated electron transport chains, they rely on simple hydrogen peroxide as the stoichiometric oxidant. Their poor robustness against H2O2 can be addressed via in situ generation of H2O2. Here we report that simple graphitic carbon nitride (g-C3N4) is a promising photocatalyst to drive peroxygenase-catalyzed hydroxylation reactions. The system has been characterized by outlining not only its scope but also its current limitations. In particular, spatial separation of the photocatalyst from the enzyme is shown as a solution to circumvent the undesired inactivation of the biocatalyst. Overall, very promising turnover numbers of the biocatalyst of more than 60.000 have been achieved.

KW - cascade reactions

KW - enzyme catalysis

KW - oxidation

KW - oxyfunctionalization

KW - photocatalysis

UR - http://www.scopus.com/inward/record.url?scp=85071061975&partnerID=8YFLogxK

U2 - 10.1021/acscatal.9b01341

DO - 10.1021/acscatal.9b01341

M3 - Article

AN - SCOPUS:85071061975

SN - 2155-5435

VL - 9

SP - 7409

EP - 7417

JO - ACS Catalysis

JF - ACS Catalysis

IS - 8

ER -

Cascading g-C₃N₄ and Peroxygenases for Selective Oxyfunctionalization Reactions

Abstract

Keywords

Access to Document

Other files and links

Fingerprint

Cite this