Communication
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Scheme 1 His and Arg based catalophore in MBH reaction.
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cyclohexenone 2 and p-bromobenzaldehyde. All the versatile
catalysts from a repository of MBH reaction24 (DBU, DABCO,
DBN, Et3N, PPh3, DMAP, His) resulted in 0–5% conversion to
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and 79% conversions (3l, Scheme 1).
The culmination of new enzymatic activity for non-natural
transformations has relied on directed evolution by protein
engineering. The focus has been to reconstruct the pre-existing
protein domains. The key to success of the present report is
hinged on the choice of catalophore and order of protein
assembly. The latter is likely to provide an organic environment
that can enhance the local concentration of substrates or render
catalophore at the interface of two proteins or both. We have
demonstrated that suitably spaced His and Arg residues can
offer to serve as the catalytic site for efficient nucleophilic
catalysis in MBH reaction. The results emphasize on controlling
the oligomeric state of the protein involved in catalysis. This
report will draw attention towards harvesting synergy of catal-
ysis and protein self-assembly that can capably offer adaptive
systems and expand the spectrum of biocatalysis.
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Acknowledgements
P. N. J., L. P. and N. K. D. are recipient of research fellowship
from CSIR and UGC, India. V. R. is a Ramanujan Fellow (SERB,
India). The authors are thankful to SERB, DAE and DBT, India
for research grants.
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Notes and references
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