Hybrid Chemo-, Bio-, and Electrocatalysis for Atom-Efficient Deuteration of Cofactors in Heavy Water
نویسندگان
چکیده
Deuterium-labeled nicotinamide cofactors such as [4-2H]-NADH can be used mechanistic probes in biological redox processes and offer a route to the synthesis of selectively [2H] labeled chemicals via biocatalytic reductive deuteration. Atom-efficient routes formation recycling are therefore highly desirable but require careful design order alleviate requirement for [2H]-labeled reducing agents. In this work, we explore suite electrode or hydrogen gas driven catalyst systems generation consider their use driving deuteration reactions. Catalysts evaluated chemoselectivity, stereoselectivity, isotopic selectivity, it is shown that inclusion an electronically coupled NAD+-reducing enzyme delivers considerable advantages over purely metal based systems, yielding exclusively [4S-2H]-NADH. We further demonstrate applicability these types [4S-2H]-NADH reactions, regardless facioselectivity enzyme.
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ژورنال
عنوان ژورنال: ACS Catalysis
سال: 2021
ISSN: ['2155-5435']
DOI: https://doi.org/10.1021/acscatal.0c03437