BIOPHYSICS. Response to Comments on "Extreme electric fields power catalysis in the active site of ketosteroid isomerase"

Science
Stephen D Fried, Steven G Boxer

Abstract

Natarajan et al. and Chen and Savidge comment that comparing the electric field in ketosteroid isomerase's (KSI's) active site to zero overestimates the catalytic effect of KSI's electric field because the reference reaction occurs in water, which itself exerts a sizable electrostatic field. To compensate, Natarajan et al. argue that additional catalytic weight arises from positioning of the general base, whereas Chen and Savidge propose a separate contribution from desolvation of the general base. We note that the former claim is not well supported by published results, and the latter claim is intriguing but lacks experimental basis. We also take the opportunity to clarify some of the more conceptually subtle aspects of electrostatic catalysis.

References

Apr 1, 1985·Proceedings of the National Academy of Sciences of the United States of America·M J Dewar, D M Storch
Aug 10, 2006·Chemical Reviews·Arieh WarshelMats H M Olsson
Oct 23, 2009·Proceedings of the National Academy of Sciences of the United States of America·Erik W DeblerIan A Wilson
Sep 29, 2011·Proceedings of the National Academy of Sciences of the United States of America·Santosh Kumar JhaSteven G Boxer
Feb 24, 2012·Proceedings of the National Academy of Sciences of the United States of America·Heidi K PrivettStephen L Mayo
Jun 27, 2013·Proceedings of the National Academy of Sciences of the United States of America·Jason P SchwansDaniel Herschlag
Mar 24, 2015·Accounts of Chemical Research·Stephen D Fried, Steven G Boxer

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Citations

Jan 20, 2017·Journal of Chemical Theory and Computation·Wiktor BekerW Andrzej Sokalski
Apr 7, 2017·Journal of the American Chemical Society·Asmit BhowmickTeresa Head-Gordon
Apr 5, 2017·Annual Review of Biochemistry·Stephen D Fried, Steven G Boxer
Dec 15, 2020·The Journal of Physical Chemistry. B·Matthias Heyden, Dmitry V Matyushov
Oct 3, 2018·Chemical Reviews·Valerie Vaissier Welborn, Teresa Head-Gordon
Jul 8, 2020·The Journal of Physical Chemistry Letters·Daniel R Martin, Dmitry V Matyushov

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