Artificial iron hydrogenase made by covalent grafting of Knölker's complex into xylanase: Application in asymmetric hydrogenation of an aryl ketone in water.

Biotechnology and Applied Biochemistry
Kalani KariyawasamRémy Ricoux

Abstract

We report a new artificial hydrogenase made by covalent anchoring of the iron Knölker's complex to a xylanase S212C variant. This artificial metalloenzyme was found to be able to catalyze efficiently the transfer hydrogenation of the benchmark substrate trifluoroacetophenone by sodium formate in water, yielding the corresponding secondary alcohol as a racemic. The reaction proceeded more than threefold faster with the XlnS212CK biohybrid than with the Knölker's complex alone. In addition, efficient conversion of trifluoroacetophenone to its corresponding alcohol was reached within 60 H with XlnS212CK, whereas a ≈2.5-fold lower conversion was observed with Knölker's complex alone as catalyst. Moreover, the data were rationalized with a computational strategy suggesting the key factors of the selectivity. These results suggested that the Knölker's complex was most likely flexible and could experience free rotational reorientation within the active-site pocket of Xln A, allowing it to access the subsite pocket populated by trifluoroacetophenone.

References

Feb 19, 2002·Chemical Reviews·Takeshi NaotaShun-Ichi Murahashi
May 1, 1959·Archives of Biochemistry and Biophysics·G L ELLMAN
Mar 18, 2005·Proceedings of the National Academy of Sciences of the United States of America·Christophe LetondorThomas R Ward
May 26, 2006·Journal of Medicinal Chemistry·René Thomsen, Mikael H Christensen
Jul 31, 2009·Organic & Biomolecular Chemistry·Rémy RicouxJean-Pierre Mahy
May 14, 2010·Nucleic Acids Research·Florian LauckTanja Kortemme
Dec 23, 2011·Chembiochem : a European Journal of Chemical Biology·Mathieu AllardRémy Ricoux
Jul 18, 2017·Chemical Reviews·Fabian SchwizerThomas R Ward
Mar 1, 2018·Chemistry : a European Journal·Alexis LatorJean-Luc Renaud
May 16, 2018·Nucleic Acids Research·Aleksander KuriataSebastian Kmiecik

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Citations

Aug 25, 2020·Biotechnology and Applied Biochemistry·Angela LombardiLong Liu

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