TY  - JOUR
A1  - Sun, Zhiyong
A1  - Glebe, Ulrich
A1  - Charan, Himanshu
A1  - Böker, Alexander
A1  - Wu, Changzhu
T1  - Enzyme-Polymer Conjugates as Robust Pickering Interfacial Biocatalysts for Efficient Biotransformations and One-Pot Cascade Reactions
JF  - Angewandte Chemie : a journal of the Gesellschaft Deutscher Chemiker ; International edition
N2  - Despite the rapid development of Pickering interfacial catalysis (PIC) at liquid-liquid interfaces with chemocatalysts, the use of unstable biocatalysts at emulsion interfaces remains a technical challenge. Herein, we present a Pickering interfacial biocatalysis (PIB) platform based on robust and recyclable enzyme-polymer conjugates that act as both catalytic sites and stabilizers at the interface of Pickering emulsions. The conjugates were prepared by growing poly(N-isopropylacrylamide) on a fragile enzyme, benzaldehyde lyase, under physiological conditions. The mild in situ conjugation process preserved the enzyme structure, and the conjugates were used to emulsify a water-organic two-phase system into a stable Pickering emulsion, leading to a significantly larger interfacial area and a 270-fold improvement in catalytic performance as compared to the unemulsified two-phase system. The PIB system could be reused multiple times. Conjugates of other enzymes were also fabricated and applied for cascade reactions.
KW  - biphasic catalysis
KW  - cascade reactions
KW  - enzyme catalysis
KW  - enzyme-polymer conjugates
KW  - Pickering interfacial catalysis
Y1  - 2018
U6  - https://doi.org/10.1002/anie.201806049
SN  - 1433-7851
SN  - 1521-3773
VL  - 57
IS  - 42
SP  - 13810
EP  - 13814
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Herter, Susanne
A1  - McKenna, Shane M.
A1  - Frazer, Andrew R.
A1  - Leimkühler, Silke
A1  - Carnell, Andrew J.
A1  - Turner, Nicholas J.
T1  - Galactose Oxidase Variants for the Oxidation of Amino Alcohols in Enzyme Cascade Synthesis
JF  - ChemCatChem : heterogeneous & homogeneous & bio- & nano-catalysis ; a journal of ChemPubSoc Europe
N2  - The use of selected engineered galactose oxidase (GOase) variants for the oxidation of amino alcohols to aldehydes under mild conditions in aqueous systems is reported. GOase variant F-2 catalyses the regioselective oxidation of N-carbobenzyloxy (Cbz)-protected 3-amino-1,2-propanediol to the corresponding -hydroxyaldehyde which was then used in an aldolase reaction. Another variant, M3-5, was found to exhibit activity towards free and N-Cbz-protected aliphatic and aromatic amino alcohols allowing the synthesis of lactams such as 3,4-dihydronaphthalen-1(2H)-one, 2-pyrrolidone and valerolactam in one-pot tandem reactions with xanthine dehydrogenase (XDH) or aldehyde oxidase (PaoABC).
KW  - aldehyde oxidase
KW  - amino alcohols
KW  - cascade reactions
KW  - enzyme catalysis
KW  - lactams
Y1  - 2015
U6  - https://doi.org/10.1002/cctc.201500218
SN  - 1867-3880
SN  - 1867-3899
VL  - 7
IS  - 15
SP  - 2313
EP  - 2317
PB  - Wiley-VCH
CY  - Weinheim
ER  -