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Mass spectrometric identification of intermediates in the O 2 -driven [4Fe-4S] to [2Fe-2S] cluster conversion in FNR
The iron-sulfur cluster containing protein Fumarate and Nitrate Reduction (FNR) is the master regulator for the switch between anaerobic and aerobic respiration in and many other bacteria. The [4Fe-4S] cluster functions as the sensory module, undergoing reaction with O that leads to conversion to a...
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| Published in: | Proceedings of the National Academy of Sciences - PNAS 2017-04, Vol.114 (16), p.E3215 |
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| Main Authors: | , , |
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| Language: | English |
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| cites | cdi_FETCH-LOGICAL-c235t-57546a56ecd9b7816fdca684d0b76cd916efd64bf8669001fa2ba84749ac689b3 |
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| container_issue | 16 |
| container_start_page | E3215 |
| container_title | Proceedings of the National Academy of Sciences - PNAS |
| container_volume | 114 |
| creator | Crack, Jason C Thomson, Andrew J Le Brun, Nick E |
| description | The iron-sulfur cluster containing protein Fumarate and Nitrate Reduction (FNR) is the master regulator for the switch between anaerobic and aerobic respiration in
and many other bacteria. The [4Fe-4S] cluster functions as the sensory module, undergoing reaction with O
that leads to conversion to a [2Fe-2S] form with loss of high-affinity DNA binding. Here, we report studies of the FNR cluster conversion reaction using time-resolved electrospray ionization mass spectrometry. The data provide insight into the reaction, permitting the detection of cluster conversion intermediates and products, including a [3Fe-3S] cluster and persulfide-coordinated [2Fe-2S] clusters [[2Fe-2S](S)
, where
= 1 or 2]. Analysis of kinetic data revealed a branched mechanism in which cluster sulfide oxidation occurs in parallel with cluster conversion and not as a subsequent, secondary reaction to generate [2Fe-2S](S)
species. This methodology shows great potential for broad application to studies of protein cofactor-small molecule interactions. |
| doi_str_mv | 10.1073/pnas.1620987114 |
| format | article |
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and many other bacteria. The [4Fe-4S] cluster functions as the sensory module, undergoing reaction with O
that leads to conversion to a [2Fe-2S] form with loss of high-affinity DNA binding. Here, we report studies of the FNR cluster conversion reaction using time-resolved electrospray ionization mass spectrometry. The data provide insight into the reaction, permitting the detection of cluster conversion intermediates and products, including a [3Fe-3S] cluster and persulfide-coordinated [2Fe-2S] clusters [[2Fe-2S](S)
, where
= 1 or 2]. Analysis of kinetic data revealed a branched mechanism in which cluster sulfide oxidation occurs in parallel with cluster conversion and not as a subsequent, secondary reaction to generate [2Fe-2S](S)
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and many other bacteria. The [4Fe-4S] cluster functions as the sensory module, undergoing reaction with O
that leads to conversion to a [2Fe-2S] form with loss of high-affinity DNA binding. Here, we report studies of the FNR cluster conversion reaction using time-resolved electrospray ionization mass spectrometry. The data provide insight into the reaction, permitting the detection of cluster conversion intermediates and products, including a [3Fe-3S] cluster and persulfide-coordinated [2Fe-2S] clusters [[2Fe-2S](S)
, where
= 1 or 2]. Analysis of kinetic data revealed a branched mechanism in which cluster sulfide oxidation occurs in parallel with cluster conversion and not as a subsequent, secondary reaction to generate [2Fe-2S](S)
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and many other bacteria. The [4Fe-4S] cluster functions as the sensory module, undergoing reaction with O
that leads to conversion to a [2Fe-2S] form with loss of high-affinity DNA binding. Here, we report studies of the FNR cluster conversion reaction using time-resolved electrospray ionization mass spectrometry. The data provide insight into the reaction, permitting the detection of cluster conversion intermediates and products, including a [3Fe-3S] cluster and persulfide-coordinated [2Fe-2S] clusters [[2Fe-2S](S)
, where
= 1 or 2]. Analysis of kinetic data revealed a branched mechanism in which cluster sulfide oxidation occurs in parallel with cluster conversion and not as a subsequent, secondary reaction to generate [2Fe-2S](S)
species. This methodology shows great potential for broad application to studies of protein cofactor-small molecule interactions.</abstract><cop>United States</cop><pmid>28373574</pmid><doi>10.1073/pnas.1620987114</doi><orcidid>https://orcid.org/0000-0001-9780-4061</orcidid><oa>free_for_read</oa></addata></record> |
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| source | JSTOR Archival Journals and Primary Sources Collection; PubMed Central |
| title | Mass spectrometric identification of intermediates in the O 2 -driven [4Fe-4S] to [2Fe-2S] cluster conversion in FNR |
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