Octahedral Trifluoromagnesate, an Anomalous Metal Fluoride Species, Stabilizes the Transition State in a Biological Motor

[Image: see text] Isoelectronic metal fluoride transition state analogue (TSA) complexes, MgF(3)(–) and AlF(4)(–), have proven to be immensely useful in understanding mechanisms of biological motors utilizing phosphoryl transfer. Here we report a previously unobserved octahedral TSA complex, MgF(3)(...

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Autores principales: Ge, Mengyu, Molt, Robert W., Jenkins, Huw T., Blackburn, G. Michael, Jin, Yi, Antson, Alfred A.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2021
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7944477/
https://www.ncbi.nlm.nih.gov/pubmed/33717640
http://dx.doi.org/10.1021/acscatal.0c04500
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author Ge, Mengyu
Molt, Robert W.
Jenkins, Huw T.
Blackburn, G. Michael
Jin, Yi
Antson, Alfred A.
author_facet Ge, Mengyu
Molt, Robert W.
Jenkins, Huw T.
Blackburn, G. Michael
Jin, Yi
Antson, Alfred A.
author_sort Ge, Mengyu
collection PubMed
description [Image: see text] Isoelectronic metal fluoride transition state analogue (TSA) complexes, MgF(3)(–) and AlF(4)(–), have proven to be immensely useful in understanding mechanisms of biological motors utilizing phosphoryl transfer. Here we report a previously unobserved octahedral TSA complex, MgF(3)(H(2)O)(−), in a 1.5 Å resolution Zika virus NS3 helicase crystal structure. (19)F NMR provided independent validation and also the direct observation of conformational tightening resulting from ssRNA binding in solution. The TSA stabilizes the two conformations of motif V of the helicase that link ATP hydrolysis with mechanical work. DFT analysis further validated the MgF(3)(H(2)O)(−) species, indicating the significance of this TSA for studies of biological motors.
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spelling pubmed-79444772021-03-11 Octahedral Trifluoromagnesate, an Anomalous Metal Fluoride Species, Stabilizes the Transition State in a Biological Motor Ge, Mengyu Molt, Robert W. Jenkins, Huw T. Blackburn, G. Michael Jin, Yi Antson, Alfred A. ACS Catal [Image: see text] Isoelectronic metal fluoride transition state analogue (TSA) complexes, MgF(3)(–) and AlF(4)(–), have proven to be immensely useful in understanding mechanisms of biological motors utilizing phosphoryl transfer. Here we report a previously unobserved octahedral TSA complex, MgF(3)(H(2)O)(−), in a 1.5 Å resolution Zika virus NS3 helicase crystal structure. (19)F NMR provided independent validation and also the direct observation of conformational tightening resulting from ssRNA binding in solution. The TSA stabilizes the two conformations of motif V of the helicase that link ATP hydrolysis with mechanical work. DFT analysis further validated the MgF(3)(H(2)O)(−) species, indicating the significance of this TSA for studies of biological motors. American Chemical Society 2021-02-17 2021-03-05 /pmc/articles/PMC7944477/ /pubmed/33717640 http://dx.doi.org/10.1021/acscatal.0c04500 Text en © 2021 The Authors. Published by American Chemical Society This is an open access article published under an ACS AuthorChoice License (https://creativecommons.org/licenses/by/4.0/) , which permits copying and redistribution of the article or any adaptations for non-commercial purposes.
spellingShingle Ge, Mengyu
Molt, Robert W.
Jenkins, Huw T.
Blackburn, G. Michael
Jin, Yi
Antson, Alfred A.
Octahedral Trifluoromagnesate, an Anomalous Metal Fluoride Species, Stabilizes the Transition State in a Biological Motor
title Octahedral Trifluoromagnesate, an Anomalous Metal Fluoride Species, Stabilizes the Transition State in a Biological Motor
title_full Octahedral Trifluoromagnesate, an Anomalous Metal Fluoride Species, Stabilizes the Transition State in a Biological Motor
title_fullStr Octahedral Trifluoromagnesate, an Anomalous Metal Fluoride Species, Stabilizes the Transition State in a Biological Motor
title_full_unstemmed Octahedral Trifluoromagnesate, an Anomalous Metal Fluoride Species, Stabilizes the Transition State in a Biological Motor
title_short Octahedral Trifluoromagnesate, an Anomalous Metal Fluoride Species, Stabilizes the Transition State in a Biological Motor
title_sort octahedral trifluoromagnesate, an anomalous metal fluoride species, stabilizes the transition state in a biological motor
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7944477/
https://www.ncbi.nlm.nih.gov/pubmed/33717640
http://dx.doi.org/10.1021/acscatal.0c04500
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