{Although|Even though|Though|Despite the fact that|While} biological iron-sulfur (Fe–S) clusters {perform|carry out|execute} {some of|a few of|a number of} {the most|probably the most|essentially the most|one of the most|by far the most} {difficult|tough|challenging|hard|tricky|complicated} redox reactions in Nature, {they are|they’re|they may be} {thought|believed} {to be|to become} composed exclusively of Fe2+ and Fe3+ ions, {as well as|in addition to|along with|and also|together with|and} mixed-valent pairs with {average|typical} oxidation states of Fe2.5+. We herein show that Fe–S clusters formally composed {of these|of those} valences can access a wider {range|variety} of electronic configurations—in {particular|specific|certain|distinct|unique}, {those|these} featuring low-valent Fe1+ centers. We demonstrate that CO binding to a synthetic [Fe4S4]0 cluster supported by N-heterocyclic carbene ligands induces generation of Fe1+ centers {via|by way of|through|by means of} intracluster electron transfer, wherein a neighboring pair of Fe2+ {sites|websites|web sites|internet sites|web-sites|web pages} reduces the CO-bound {site|website|web site|internet site|web-site|web page} to a low-valent Fe1+ state. Similarly, CO binding to an [Fe4S4]+ cluster induces electron delocalization {with a|having a|using a} neighboring Fe {site|website|web site|internet site|web-site|web page} to {form|type|kind} a mixed-valent Fe1.5+Fe2.5+ pair in which the CO-bound {site|website|web site|internet site|web-site|web page} adopts partial low-valent character. These low-valent configurations engender {remarkable|outstanding|exceptional} C–O bond activation {without having to|without needing to} traverse {highly|extremely|very|hugely} {negative|unfavorable|damaging|adverse} and physiologically inaccessible Fe2+/Fe1+ redox couples. Ethyl 5-bromo-2-methylnicotinate manufacturer Z-Asp(OtBu)-OH Order PMID:23865629
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