Cascading g-C3N4 and Peroxygenases for Selective Oxyfunctionalization Reactions

被引：72

作者：

van Schie, Morten M. C. H. ^{[1
]}

Zhang, Wuyuan ^{[1
]}

Tieves, Florian ^{[1
]}

Choi, Da Som ^{[2
]}

Park, Chan Beum ^{[2
]}

Burek, Bastien O. ^{[3
]}

Bloh, Jonathan Z. ^{[3
]}

Arends, Isabel W. C. E. ^{[4
]}

Paul, Caroline E. ^{[1
]}

Alcalde, Miguel ^{[5
]}

Hollmann, Frank ^{[1
]}

机构：

[1] Delft Univ Technol, Dept Biotechnol, Maasweg 9, NL-2629 HZ Delft, Netherlands

[2] Korea Adv Inst Sci & Technol, Dept Mat Sci & Engn, 335 Sci Rd, Daejeon 305701, South Korea

[3] DECHEMA Forschungsinst, Theodor Heuss Allee 25, D-60486 Frankfurt, Germany

[4] Univ Utrecht, Fac Sci, Budapestlaan 6, NL-3584 CD Utrecht, Netherlands

[5] CSIC, Inst Catalysis, Dept Biocatalysis, E-28049 Madrid, Spain

来源：

ACS CATALYSIS | 2019年 / 9卷 / 08期

基金：

欧盟地平线“2020”;

关键词：

cascade reactions; enzyme catalysis; oxidation; oxyfunctionalization; photocatalysis; LIPASE-MEDIATED EPOXIDATION; AMORPHOUS-CARBON NITRIDE; C-H BONDS; WATER OXIDATION; UNSPECIFIC PEROXYGENASE; HYDROGEN-PEROXIDE; H2O2; PRODUCTION; PHOTOCATALYST; HALOPEROXIDASE; INACTIVATION;

D O I：

10.1021/acscatal.9b01341

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

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.

引用

页码：7409 / 7417

页数：17

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