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2016 ; 472
(2189
): 20160078
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Proteins as templates for complex synthetic metalloclusters: towards biologically
programmed heterogeneous catalysis
#MMPMID27279776
Fehl C
; Davis BG
Proc Math Phys Eng Sci
2016[May]; 472
(2189
): 20160078
PMID27279776
show ga
Despite nature's prevalent use of metals as prosthetics to adapt or enhance the
behaviour of proteins, our ability to programme such architectural organization
remains underdeveloped. Multi-metal clusters buried in proteins underpin the most
remarkable chemical transformations in nature, but we are not yet in a position
to fully mimic or exploit such systems. With the advent of copious, relevant
structural information, judicious mechanistic studies and the use of accessible
computational methods in protein design coupled with new synthetic methods for
building biomacromolecules, we can envisage a 'new dawn' that will allow us to
build de novo metalloenzymes that move beyond mono-metal centres. In particular,
we highlight the need for systems that approach the multi-centred clusters that
have evolved to couple electron shuttling with catalysis. Such hybrids may be
viewed as exciting mid-points between homogeneous and heterogeneous catalysts
which also exploit the primary benefits of biocatalysis.