Publicação
Unusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspective
| Resumo: | The universe of known biological FeS clusters is constantly enlarging. Besides the conventional, well described [2Fe–2S], [3Fe–4S] and cubane [4Fe–4S] clusters, novel, unprecedented structures are emerging. They include unusually coordinated clusters, with additional sulfur atoms, e.g., [4Fe–5S], [5Fe–5S], [4Fe–4S]-5S-[4Fe–4S], [8Fe–7S], [8Fe–9S] and [8Fe–8S–C] and heteronuclear clusters, e.g., [Ni–4Fe–4S], [2Ni–4Fe–4S], [4Fe–4S]-[2Ru], [Me–7Fe–9S–C–(homocitrate)] that undertake versatile physiological roles in the activation of small molecules (H2, CO2, CO and N2) and in the sulfuration of different compounds (e.g., t-RNAs, biotin and lipoic acid) in biology. A few structures are characterized by highly distorted geometries, e.g., the non-cubane [4Fe–4S] center and the hydrogenase-related [4Fe–3S] cluster, and contain atypical ligations or vacant coordination sites, which confer them novel functions far from the common electron transfer. Herein, we single out clusters found in i) hydrogenases that ensure sustainable hydrogen cycling, promising a clean fuel production in the future, ii) radical-SAM enzymes that can inspire applied catalysis due to an intrinsic flexibility of the radical chemistry, and iii) standard [4Fe–4S] cluster with still unknown function in DNA repair enzymes, which offer a possibility to interfere with DNA repair in pathogens or improve it in humans. Focusing on the abovementioned enzymes, we demonstrate the unique power of resonance Raman spectroscopy to unveil remarkable features in FeS centers, which has contributed to our understanding of unusual structures and disentangling of unknown functions. |
|---|---|
| Autores principais: | Caserta, Giorgio |
| Outros Autores: | Zuccarello, Lidia; Barbosa, Catarina; Silveira, Célia M.; Moe, Elin; Katz, Sagie; Hildebrandt, Peter; Zebger, Ingo; Todorovic, Smilja |
| Assunto: | FeS clusters Glycosylase Hydrogenase Radical-SAM Resonance Raman spectroscopy Physical and Theoretical Chemistry Inorganic Chemistry Materials Chemistry SDG 7 - Affordable and Clean Energy |
| Ano: | 2022 |
| País: | Portugal |
| Tipo de documento: | recensão |
| Tipo de acesso: | acesso aberto |
| Instituição associada: | Universidade Nova de Lisboa |
| Idioma: | inglês |
| Origem: | Repositório Institucional da UNL |
| _version_ | 1868982861159202816 |
|---|---|
| author | Caserta, Giorgio |
| author2 | Zuccarello, Lidia Barbosa, Catarina Silveira, Célia M. Moe, Elin Katz, Sagie Hildebrandt, Peter Zebger, Ingo Todorovic, Smilja |
| author2_role | author author author author author author author author |
| author_facet | Caserta, Giorgio Zuccarello, Lidia Barbosa, Catarina Silveira, Célia M. Moe, Elin Katz, Sagie Hildebrandt, Peter Zebger, Ingo Todorovic, Smilja |
| author_role | author |
| contributor_name_str_mv | Instituto de Tecnologia Química e Biológica António Xavier (ITQB) Elsevier RUN |
| country_str | PT |
| creators_json_txt | [{\"Person.name\":\"Caserta, Giorgio\"},{\"Person.name\":\"Zuccarello, Lidia\"},{\"Person.name\":\"Barbosa, Catarina\"},{\"Person.name\":\"Silveira, Célia M.\"},{\"Person.name\":\"Moe, Elin\"},{\"Person.name\":\"Katz, Sagie\"},{\"Person.name\":\"Hildebrandt, Peter\"},{\"Person.name\":\"Zebger, Ingo\"},{\"Person.name\":\"Todorovic, Smilja\"}] |
| datacite.contributors.contributor.contributorName.fl_str_mv | Instituto de Tecnologia Química e Biológica António Xavier (ITQB) Elsevier RUN |
| datacite.creators.creator.creatorName.fl_str_mv | Caserta, Giorgio Zuccarello, Lidia Barbosa, Catarina Silveira, Célia M. Moe, Elin Katz, Sagie Hildebrandt, Peter Zebger, Ingo Todorovic, Smilja |
| datacite.date.Accepted.fl_str_mv | 2022-02-01T00:00:00Z |
| datacite.date.available.fl_str_mv | 2022-07-20T22:30:47Z |
| datacite.date.embargoed.fl_str_mv | 2022-07-20T22:30:47Z |
| datacite.rights.fl_str_mv | http://purl.org/coar/access_right/c_abf2 |
| datacite.subjects.subject.fl_str_mv | FeS clusters Glycosylase Hydrogenase Radical-SAM Resonance Raman spectroscopy Physical and Theoretical Chemistry Inorganic Chemistry Materials Chemistry SDG 7 - Affordable and Clean Energy |
| datacite.titles.title.fl_str_mv | Unusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspective |
| dc.contributor.none.fl_str_mv | Instituto de Tecnologia Química e Biológica António Xavier (ITQB) Elsevier RUN |
| dc.creator.none.fl_str_mv | Caserta, Giorgio Zuccarello, Lidia Barbosa, Catarina Silveira, Célia M. Moe, Elin Katz, Sagie Hildebrandt, Peter Zebger, Ingo Todorovic, Smilja |
| dc.date.Accepted.fl_str_mv | 2022-02-01T00:00:00Z |
| dc.date.available.fl_str_mv | 2022-07-20T22:30:47Z |
| dc.date.embargoed.fl_str_mv | 2022-07-20T22:30:47Z |
| dc.format.none.fl_str_mv | application/pdf |
| dc.identifier.none.fl_str_mv | http://hdl.handle.net/10362/142219 |
| dc.language.none.fl_str_mv | eng |
| dc.rights.none.fl_str_mv | http://purl.org/coar/access_right/c_abf2 |
| dc.subject.none.fl_str_mv | FeS clusters Glycosylase Hydrogenase Radical-SAM Resonance Raman spectroscopy Physical and Theoretical Chemistry Inorganic Chemistry Materials Chemistry SDG 7 - Affordable and Clean Energy |
| dc.title.fl_str_mv | Unusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspective |
| dc.type.none.fl_str_mv | http://purl.org/coar/resource_type/c_efa0 |
| description | The universe of known biological FeS clusters is constantly enlarging. Besides the conventional, well described [2Fe–2S], [3Fe–4S] and cubane [4Fe–4S] clusters, novel, unprecedented structures are emerging. They include unusually coordinated clusters, with additional sulfur atoms, e.g., [4Fe–5S], [5Fe–5S], [4Fe–4S]-5S-[4Fe–4S], [8Fe–7S], [8Fe–9S] and [8Fe–8S–C] and heteronuclear clusters, e.g., [Ni–4Fe–4S], [2Ni–4Fe–4S], [4Fe–4S]-[2Ru], [Me–7Fe–9S–C–(homocitrate)] that undertake versatile physiological roles in the activation of small molecules (H2, CO2, CO and N2) and in the sulfuration of different compounds (e.g., t-RNAs, biotin and lipoic acid) in biology. A few structures are characterized by highly distorted geometries, e.g., the non-cubane [4Fe–4S] center and the hydrogenase-related [4Fe–3S] cluster, and contain atypical ligations or vacant coordination sites, which confer them novel functions far from the common electron transfer. Herein, we single out clusters found in i) hydrogenases that ensure sustainable hydrogen cycling, promising a clean fuel production in the future, ii) radical-SAM enzymes that can inspire applied catalysis due to an intrinsic flexibility of the radical chemistry, and iii) standard [4Fe–4S] cluster with still unknown function in DNA repair enzymes, which offer a possibility to interfere with DNA repair in pathogens or improve it in humans. Focusing on the abovementioned enzymes, we demonstrate the unique power of resonance Raman spectroscopy to unveil remarkable features in FeS centers, which has contributed to our understanding of unusual structures and disentangling of unknown functions. |
| dirty | 0 |
| eu_rights_str_mv | openAccess |
| format | review |
| fulltext.url.fl_str_mv | https://run.unl.pt/bitstreams/01d0cd10-c880-42aa-9b17-d0815e4fa029/download |
| id | run_9dd429ec6bd17954f7d2efb1c63c8d80 |
| identifier.url.fl_str_mv | http://hdl.handle.net/10362/142219 |
| inst_facet_str | urn:organizationAcronym:unl{{{_:::_}}}Universidade Nova de Lisboa |
| instacron_str | unl |
| institution | Universidade Nova de Lisboa |
| instname_str | Universidade Nova de Lisboa |
| language | eng |
| network_acronym_str | run |
| network_name_str | Repositório Institucional da UNL |
| oai_identifier_str | oai:run.unl.pt:10362/142219 |
| organization_str_mv | urn:organizationAcronym:unl |
| person_str_mv | Caserta, Giorgio Zuccarello, Lidia Barbosa, Catarina Silveira, Célia M. Moe, Elin Katz, Sagie Hildebrandt, Peter Zebger, Ingo Todorovic, Smilja |
| publishDate | 2022 |
| repo_facet_str | urn:repositoryAcronym:run{{{_:::_}}}Repositório Institucional da UNL |
| reponame_str | Repositório Institucional da UNL |
| repository_id_str | urn:repositoryAcronym:run |
| service_str_mv | urn:repositoryAcronym:run |
| spelling | engenThe universe of known biological FeS clusters is constantly enlarging. Besides the conventional, well described [2Fe–2S], [3Fe–4S] and cubane [4Fe–4S] clusters, novel, unprecedented structures are emerging. They include unusually coordinated clusters, with additional sulfur atoms, e.g., [4Fe–5S], [5Fe–5S], [4Fe–4S]-5S-[4Fe–4S], [8Fe–7S], [8Fe–9S] and [8Fe–8S–C] and heteronuclear clusters, e.g., [Ni–4Fe–4S], [2Ni–4Fe–4S], [4Fe–4S]-[2Ru], [Me–7Fe–9S–C–(homocitrate)] that undertake versatile physiological roles in the activation of small molecules (H2, CO2, CO and N2) and in the sulfuration of different compounds (e.g., t-RNAs, biotin and lipoic acid) in biology. A few structures are characterized by highly distorted geometries, e.g., the non-cubane [4Fe–4S] center and the hydrogenase-related [4Fe–3S] cluster, and contain atypical ligations or vacant coordination sites, which confer them novel functions far from the common electron transfer. Herein, we single out clusters found in i) hydrogenases that ensure sustainable hydrogen cycling, promising a clean fuel production in the future, ii) radical-SAM enzymes that can inspire applied catalysis due to an intrinsic flexibility of the radical chemistry, and iii) standard [4Fe–4S] cluster with still unknown function in DNA repair enzymes, which offer a possibility to interfere with DNA repair in pathogens or improve it in humans. Focusing on the abovementioned enzymes, we demonstrate the unique power of resonance Raman spectroscopy to unveil remarkable features in FeS centers, which has contributed to our understanding of unusual structures and disentangling of unknown functions.application/pdfenUnusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspectiveCaserta, GiorgioZuccarello, LidiaBarbosa, CatarinaSilveira, Célia M.Moe, ElinKatz, SagieHildebrandt, PeterZebger, IngoTodorovic, SmiljaInstituto de Tecnologia Química e Biológica António Xavier (ITQB)ElsevierHostingInstitutionOrganizationalRUNe-mailmailto:run@unl.ptrun@unl.ptISSNIsPartOf0010-8545URNIsPartOfPURE: 43574064URNIsPartOfPURE UUID: 3a12ad12-ad2c-402b-a7e2-ee729e219d57URNIsPartOfScopus: 85118884484DOIIsPartOf10.1016/j.ccr.2021.2142872022-07-20T22:30:47Z2022-02-012022-02-01T00:00:00ZHandlehttp://hdl.handle.net/10362/142219http://purl.org/coar/access_right/c_abf2open accessFeS clustersGlycosylaseHydrogenaseRadical-SAMResonance Raman spectroscopyPhysical and Theoretical ChemistryInorganic ChemistryMaterials ChemistrySDG 7 - Affordable and Clean Energy2241708 bytesother research producthttp://purl.org/coar/resource_type/c_efa0reviewhttp://purl.org/coar/access_right/c_abf2application/pdffulltexthttps://run.unl.pt/bitstreams/01d0cd10-c880-42aa-9b17-d0815e4fa029/download |
| spellingShingle | Unusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspective Caserta, Giorgio FeS clusters Glycosylase Hydrogenase Radical-SAM Resonance Raman spectroscopy Physical and Theoretical Chemistry Inorganic Chemistry Materials Chemistry SDG 7 - Affordable and Clean Energy |
| status | SINGLETON |
| subject.fl_str_mv | FeS clusters Glycosylase Hydrogenase Radical-SAM Resonance Raman spectroscopy Physical and Theoretical Chemistry Inorganic Chemistry Materials Chemistry SDG 7 - Affordable and Clean Energy |
| title | Unusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspective |
| title_full | Unusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspective |
| title_fullStr | Unusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspective |
| title_full_unstemmed | Unusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspective |
| title_short | Unusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspective |
| title_sort | Unusual structures and unknown roles of FeS clusters in metalloenzymes seen from a resonance Raman spectroscopic perspective |
| topic | FeS clusters Glycosylase Hydrogenase Radical-SAM Resonance Raman spectroscopy Physical and Theoretical Chemistry Inorganic Chemistry Materials Chemistry SDG 7 - Affordable and Clean Energy |
| topic_facet | FeS clusters Glycosylase Hydrogenase Radical-SAM Resonance Raman spectroscopy Physical and Theoretical Chemistry Inorganic Chemistry Materials Chemistry SDG 7 - Affordable and Clean Energy |
| url | http://hdl.handle.net/10362/142219 |
| visible | 1 |