Inhibition of [FeFe]-hydrogenases by formaldehyde and wider mechanistic implications for biohydrogen activation.
Formaldehyde-a rapid and reversible inhibitor of hydrogen evolution by [FeFe]-hydrogenases-binds with a strong potential dependence that is almost complementary to that of CO. Whereas exogenous CO binds tightly to the oxidized state known as H(ox) but very weakly to a state two electrons more reduce...
Main Authors: | , , , , , , , |
---|---|
Format: | Journal article |
Language: | English |
Published: |
2012
|
_version_ | 1826278950894043136 |
---|---|
author | Foster, C Krämer, T Wait, A Parkin, A Jennings, D Happe, T McGrady, J Armstrong, F |
author_facet | Foster, C Krämer, T Wait, A Parkin, A Jennings, D Happe, T McGrady, J Armstrong, F |
author_sort | Foster, C |
collection | OXFORD |
description | Formaldehyde-a rapid and reversible inhibitor of hydrogen evolution by [FeFe]-hydrogenases-binds with a strong potential dependence that is almost complementary to that of CO. Whereas exogenous CO binds tightly to the oxidized state known as H(ox) but very weakly to a state two electrons more reduced, formaldehyde interacts most strongly with the latter. Formaldehyde thus intercepts increasingly reduced states of the catalytic cycle, and density functional theory calculations support the proposal that it reacts with the H-cluster directly, most likely targeting an otherwise elusive and highly reactive Fe-hydrido (Fe-H) intermediate. |
first_indexed | 2024-03-06T23:51:34Z |
format | Journal article |
id | oxford-uuid:72c7fd66-16c6-4260-857b-0dbe67becedb |
institution | University of Oxford |
language | English |
last_indexed | 2024-03-06T23:51:34Z |
publishDate | 2012 |
record_format | dspace |
spelling | oxford-uuid:72c7fd66-16c6-4260-857b-0dbe67becedb2022-03-26T19:52:17ZInhibition of [FeFe]-hydrogenases by formaldehyde and wider mechanistic implications for biohydrogen activation.Journal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:72c7fd66-16c6-4260-857b-0dbe67becedbEnglishSymplectic Elements at Oxford2012Foster, CKrämer, TWait, AParkin, AJennings, DHappe, TMcGrady, JArmstrong, FFormaldehyde-a rapid and reversible inhibitor of hydrogen evolution by [FeFe]-hydrogenases-binds with a strong potential dependence that is almost complementary to that of CO. Whereas exogenous CO binds tightly to the oxidized state known as H(ox) but very weakly to a state two electrons more reduced, formaldehyde interacts most strongly with the latter. Formaldehyde thus intercepts increasingly reduced states of the catalytic cycle, and density functional theory calculations support the proposal that it reacts with the H-cluster directly, most likely targeting an otherwise elusive and highly reactive Fe-hydrido (Fe-H) intermediate. |
spellingShingle | Foster, C Krämer, T Wait, A Parkin, A Jennings, D Happe, T McGrady, J Armstrong, F Inhibition of [FeFe]-hydrogenases by formaldehyde and wider mechanistic implications for biohydrogen activation. |
title | Inhibition of [FeFe]-hydrogenases by formaldehyde and wider mechanistic implications for biohydrogen activation. |
title_full | Inhibition of [FeFe]-hydrogenases by formaldehyde and wider mechanistic implications for biohydrogen activation. |
title_fullStr | Inhibition of [FeFe]-hydrogenases by formaldehyde and wider mechanistic implications for biohydrogen activation. |
title_full_unstemmed | Inhibition of [FeFe]-hydrogenases by formaldehyde and wider mechanistic implications for biohydrogen activation. |
title_short | Inhibition of [FeFe]-hydrogenases by formaldehyde and wider mechanistic implications for biohydrogen activation. |
title_sort | inhibition of fefe hydrogenases by formaldehyde and wider mechanistic implications for biohydrogen activation |
work_keys_str_mv | AT fosterc inhibitionoffefehydrogenasesbyformaldehydeandwidermechanisticimplicationsforbiohydrogenactivation AT kramert inhibitionoffefehydrogenasesbyformaldehydeandwidermechanisticimplicationsforbiohydrogenactivation AT waita inhibitionoffefehydrogenasesbyformaldehydeandwidermechanisticimplicationsforbiohydrogenactivation AT parkina inhibitionoffefehydrogenasesbyformaldehydeandwidermechanisticimplicationsforbiohydrogenactivation AT jenningsd inhibitionoffefehydrogenasesbyformaldehydeandwidermechanisticimplicationsforbiohydrogenactivation AT happet inhibitionoffefehydrogenasesbyformaldehydeandwidermechanisticimplicationsforbiohydrogenactivation AT mcgradyj inhibitionoffefehydrogenasesbyformaldehydeandwidermechanisticimplicationsforbiohydrogenactivation AT armstrongf inhibitionoffefehydrogenasesbyformaldehydeandwidermechanisticimplicationsforbiohydrogenactivation |