A Mn(salen)-Based Artificial Metalloenzyme for Nitrene and Oxene Transfer Catalysis

被引：0
作者：
Liu, Zhennan [1 ]
Law, Yee-Song [2 ]
Kumar Verma, Ravi [3 ]
Ling Goh, Yi [1 ]
Eddy Wong, Mun Fei [1 ]
Sana, Barindra [2 ]
Fan, Hao [3 ,4 ]
Lui Ang, Ee [2 ,4 ]
Hwee Lim, Yee [1 ,4 ]
机构：
[1] ASTAR, Inst Sustainabil Chem Energy & Environm ISCE2, 8 Biomed Grove,Neuros 07-01, Singapore 138665, Singapore
[2] ASTAR, Singapore Inst Food & Biotechnol Innovat SIFBI, 31 Biopolis Way,Nanos 01-02, Singapore 138669, Singapore
[3] ASTAR, Bioinformat Inst BII, 30 Biopolis St,Matrix 07-01, Singapore 138671, Singapore
[4] Natl Univ Singapore, Yong Loo Lin Sch Med, Synthet Biol Translat Res Program, 10 Med Dr, Singapore 117597, Singapore
来源：
CHEMBIOCHEM | 2025年 / 26卷 / 05期
关键词：
Metalloenzymes; Biotin-avidin technology; Aziridination; Oxidation; Schiff bases; C-H; NONHEME IRON; OXIDATION; COMPLEXES; STREPTAVIDIN; EPOXIDATION; EVOLUTION; INSIGHTS; H2O2;
D O I：
10.1002/cbic.202400774
中图分类号：
Q5 [生物化学]; Q7 [分子生物学];
学科分类号：
071010 ; 081704 ;
摘要：
The development of artificial metalloenzymes (ArMs) offers a potent approach to incorporate non-natural chemical reactions into biocatalysis. Here we report the assembly of Mn(salen)-based ArMs by embedding biotinylated Mn(salen) complexes into streptavidin (Sav) variants. Using commercially available nitrene and oxo transfer reagents, these biohybrid catalysts catalyzed the aziridination of alkenes and oxidation of benzylic C-H bonds with up to 19 and 146 turnover numbers.
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页数：6
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[1]   CHEMICAL-COMPOSITION OF THE MANTLE [J].
ANDERSON, DL .
JOURNAL OF GEOPHYSICAL RESEARCH, 1983, 88 :B41-B52
[2]  
Barynin V.V., ENCY INORGANIC BIOIN
[3]   Chloromethyl-triazole: a new motif for site-selective pseudo-acylation of proteins [J].
Brewster, Richard C. ;
Gavins, Georgina C. ;
Gunthardt, Barbara ;
Farr, Sarah ;
Webb, Kimberly M. ;
Voigt, Philipp ;
Hulme, Alison N. .
CHEMICAL COMMUNICATIONS, 2016, 52 (82) :12230-12232
[4]   A site-selective dual anchoring strategy for artificial metalloprotein design [J].
Carey, JR ;
Ma, SK ;
Pfister, TD ;
Garner, DK ;
Kim, HK ;
Abramite, JA ;
Wang, ZL ;
Guo, ZJ ;
Lu, Y .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (35) :10812-10813
[5]   Design and evolution of chimeric streptavidin for protein-enabled dual gold catalysis [J].
Christoffel, Fadri ;
Igareta, Nico, V ;
Pellizzoni, Michela M. ;
Tiessler-Sala, Laura ;
Lozhkin, Boris ;
Spiess, Daniel C. ;
Lledos, Agusti ;
Marechal, Jean-Didier ;
Peterson, Ryan L. ;
Ward, Thomas R. .
NATURE CATALYSIS, 2021, 4 (08) :643-+
[6]   PARTICLE MESH EWALD - AN N.LOG(N) METHOD FOR EWALD SUMS IN LARGE SYSTEMS [J].
DARDEN, T ;
YORK, D ;
PEDERSEN, L .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (12) :10089-10092
[7]   Artificial Metalloenzymes: Challenges and Opportunities [J].
Davis, Holly J. ;
Ward, Thomas R. .
ACS CENTRAL SCIENCE, 2019, 5 (07) :1120-1136
[8]   Artificial Transfer Hydrogenases for the Enantioselective Reduction of Cyclic Imines [J].
Duerrenberger, Marc ;
Heinisch, Tillmann ;
Wilson, Yvonne M. ;
Rossel, Thibaud ;
Nogueira, Elisa ;
Knoerr, Livia ;
Mutschler, Annette ;
Kersten, Karoline ;
Zimbron, Malcolm Jeremy ;
Pierron, Julien ;
Schirmer, Tilman ;
Ward, Thomas R. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (13) :3026-3029
[9]   CONSTANT-PRESSURE MOLECULAR-DYNAMICS SIMULATION - THE LANGEVIN PISTON METHOD [J].
FELLER, SE ;
ZHANG, YH ;
PASTOR, RW ;
BROOKS, BR .
JOURNAL OF CHEMICAL PHYSICS, 1995, 103 (11) :4613-4621
[10]   Apoenzyme Reconstitution as a Chemical Tool for Structural Enzymology and Biotechnology [J].
Fruk, Ljiljana ;
Kuo, Chi-Hsien ;
Torres, Eduardo ;
Niemeyer, Christof M. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2009, 48 (09) :1550-1574
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