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Engineering a hyper-catalytic enzyme by photo-activated conformation modulation

Journal Article · · Journal of Physical Chemistry Letters
DOI:https://doi.org/10.1021/jz201675m· OSTI ID:1049065

Enzyme engineering for improved catalysis has wide implications. We describe a novel chemical modification of Candida antarctica lipase B that allows modulation of the enzyme conformation to promote catalysis. Computational modeling was used to identify dynamical enzyme regions that impact the catalytic mechanism. Surface loop regions located distal to active site but showing dynamical coupling to the reaction were connected by a chemical bridge between Lys136 and Pro192, containing a derivative of azobenzene. The conformational modulation of the enzyme was achieved using two sources of light that alternated the azobenzene moiety in cis and trans conformations. Computational model predicted that mechanical energy from the conformational fluctuations facilitate the reaction in the active-site. The results were consistent with predictions as the activity of the engineered enzyme was found to be enhanced with photoactivation. Preliminary estimations indicate that the engineered enzyme achieved 8-52 fold better catalytic activity than the unmodulated enzyme.

Research Organization:
Oak Ridge National Laboratory (ORNL); Center for Computational Sciences
Sponsoring Organization:
ORNL LDRD Director's R&D
DOE Contract Number:
AC05-00OR22725
OSTI ID:
1049065
Journal Information:
Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 9 Vol. 3; ISSN 1948-7185
Country of Publication:
United States
Language:
English

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