%0 Journal Article %T In Vitro Production of Ergothioneine Isotopologues. %A Beliaeva MA %A Burn R %A Lim D %A Seebeck FP %J Angew Chem Int Ed Engl %V 60 %N 10 %D 03 2021 1 %M 32996678 %F 16.823 %R 10.1002/anie.202011096 %X Ergothioneine is an emerging component of the redox homeostasis system in human cells and in microbial pathogens, such as Mycobacterium tuberculosis and Burkholderia pseudomallei. The synthesis of stable isotope-labeled ergothioneine derivatives may provide important tools for deciphering the distribution, function, and metabolism of this compound in vivo. We describe a general protocol for the production of ergothioneine isotopologues with programmable 2 H, 15 N, 13 C, 34 S, and 33 S isotope labeling patterns. This enzyme-based approach makes efficient use of commercial isotope reagents and is also directly applicable to the synthesis of radio-isotopologues.