Going around the Kok cycle of the water oxidation reaction with femtosecond X-ray crystallography
The water oxidation reaction in photosystem II (PS II) produces most of the molecular oxygen in the atmosphere, which sustains life on Earth, and in this process releases four electrons and four protons that drive the downstream process of CO(2) fixation in the photosynthetic apparatus. The catalyti...
Autores principales: | , , , , , , , , , , , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
International Union of Crystallography
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10619448/ https://www.ncbi.nlm.nih.gov/pubmed/37870936 http://dx.doi.org/10.1107/S2052252523008928 |
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author | Bhowmick, Asmit Simon, Philipp S. Bogacz, Isabel Hussein, Rana Zhang, Miao Makita, Hiroki Ibrahim, Mohamed Chatterjee, Ruchira Doyle, Margaret D. Cheah, Mun Hon Chernev, Petko Fuller, Franklin D. Fransson, Thomas Alonso-Mori, Roberto Brewster, Aaron S. Sauter, Nicholas K. Bergmann, Uwe Dobbek, Holger Zouni, Athina Messinger, Johannes Kern, Jan Yachandra, Vittal K. Yano, Junko |
author_facet | Bhowmick, Asmit Simon, Philipp S. Bogacz, Isabel Hussein, Rana Zhang, Miao Makita, Hiroki Ibrahim, Mohamed Chatterjee, Ruchira Doyle, Margaret D. Cheah, Mun Hon Chernev, Petko Fuller, Franklin D. Fransson, Thomas Alonso-Mori, Roberto Brewster, Aaron S. Sauter, Nicholas K. Bergmann, Uwe Dobbek, Holger Zouni, Athina Messinger, Johannes Kern, Jan Yachandra, Vittal K. Yano, Junko |
author_sort | Bhowmick, Asmit |
collection | PubMed |
description | The water oxidation reaction in photosystem II (PS II) produces most of the molecular oxygen in the atmosphere, which sustains life on Earth, and in this process releases four electrons and four protons that drive the downstream process of CO(2) fixation in the photosynthetic apparatus. The catalytic center of PS II is an oxygen-bridged Mn(4)Ca complex (Mn(4)CaO(5)) which is progressively oxidized upon the absorption of light by the chlorophyll of the PS II reaction center, and the accumulation of four oxidative equivalents in the catalytic center results in the oxidation of two waters to dioxygen in the last step. The recent emergence of X-ray free-electron lasers (XFELs) with intense femtosecond X-ray pulses has opened up opportunities to visualize this reaction in PS II as it proceeds through the catalytic cycle. In this review, we summarize our recent studies of the catalytic reaction in PS II by following the structural changes along the reaction pathway via room-temperature X-ray crystallography using XFELs. The evolution of the electron density changes at the Mn complex reveals notable structural changes, including the insertion of O(X) from a new water molecule, which disappears on completion of the reaction, implicating it in the O—O bond formation reaction. We were also able to follow the structural dynamics of the protein coordinating with the catalytic complex and of channels within the protein that are important for substrate and product transport, revealing well orchestrated conformational changes in response to the electronic changes at the Mn(4)Ca cluster. |
format | Online Article Text |
id | pubmed-10619448 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | International Union of Crystallography |
record_format | MEDLINE/PubMed |
spelling | pubmed-106194482023-11-02 Going around the Kok cycle of the water oxidation reaction with femtosecond X-ray crystallography Bhowmick, Asmit Simon, Philipp S. Bogacz, Isabel Hussein, Rana Zhang, Miao Makita, Hiroki Ibrahim, Mohamed Chatterjee, Ruchira Doyle, Margaret D. Cheah, Mun Hon Chernev, Petko Fuller, Franklin D. Fransson, Thomas Alonso-Mori, Roberto Brewster, Aaron S. Sauter, Nicholas K. Bergmann, Uwe Dobbek, Holger Zouni, Athina Messinger, Johannes Kern, Jan Yachandra, Vittal K. Yano, Junko IUCrJ Topical Reviews The water oxidation reaction in photosystem II (PS II) produces most of the molecular oxygen in the atmosphere, which sustains life on Earth, and in this process releases four electrons and four protons that drive the downstream process of CO(2) fixation in the photosynthetic apparatus. The catalytic center of PS II is an oxygen-bridged Mn(4)Ca complex (Mn(4)CaO(5)) which is progressively oxidized upon the absorption of light by the chlorophyll of the PS II reaction center, and the accumulation of four oxidative equivalents in the catalytic center results in the oxidation of two waters to dioxygen in the last step. The recent emergence of X-ray free-electron lasers (XFELs) with intense femtosecond X-ray pulses has opened up opportunities to visualize this reaction in PS II as it proceeds through the catalytic cycle. In this review, we summarize our recent studies of the catalytic reaction in PS II by following the structural changes along the reaction pathway via room-temperature X-ray crystallography using XFELs. The evolution of the electron density changes at the Mn complex reveals notable structural changes, including the insertion of O(X) from a new water molecule, which disappears on completion of the reaction, implicating it in the O—O bond formation reaction. We were also able to follow the structural dynamics of the protein coordinating with the catalytic complex and of channels within the protein that are important for substrate and product transport, revealing well orchestrated conformational changes in response to the electronic changes at the Mn(4)Ca cluster. International Union of Crystallography 2023-10-24 /pmc/articles/PMC10619448/ /pubmed/37870936 http://dx.doi.org/10.1107/S2052252523008928 Text en © Asmit Bhowmick et al. 2023 https://creativecommons.org/licenses/by/4.0/This is an open-access article distributed under the terms of the Creative Commons Attribution (CC-BY) Licence, which permits unrestricted use, distribution, and reproduction in any medium, provided the original authors and source are cited. |
spellingShingle | Topical Reviews Bhowmick, Asmit Simon, Philipp S. Bogacz, Isabel Hussein, Rana Zhang, Miao Makita, Hiroki Ibrahim, Mohamed Chatterjee, Ruchira Doyle, Margaret D. Cheah, Mun Hon Chernev, Petko Fuller, Franklin D. Fransson, Thomas Alonso-Mori, Roberto Brewster, Aaron S. Sauter, Nicholas K. Bergmann, Uwe Dobbek, Holger Zouni, Athina Messinger, Johannes Kern, Jan Yachandra, Vittal K. Yano, Junko Going around the Kok cycle of the water oxidation reaction with femtosecond X-ray crystallography |
title | Going around the Kok cycle of the water oxidation reaction with femtosecond X-ray crystallography |
title_full | Going around the Kok cycle of the water oxidation reaction with femtosecond X-ray crystallography |
title_fullStr | Going around the Kok cycle of the water oxidation reaction with femtosecond X-ray crystallography |
title_full_unstemmed | Going around the Kok cycle of the water oxidation reaction with femtosecond X-ray crystallography |
title_short | Going around the Kok cycle of the water oxidation reaction with femtosecond X-ray crystallography |
title_sort | going around the kok cycle of the water oxidation reaction with femtosecond x-ray crystallography |
topic | Topical Reviews |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10619448/ https://www.ncbi.nlm.nih.gov/pubmed/37870936 http://dx.doi.org/10.1107/S2052252523008928 |
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