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XFEL serial crystallography reveals the room temperature structure of methyl-coenzyme M reductase

Ohmer, Christopher J. (författare)
Univ Michigan, Dept Biol Chem, Sch Med, 1150 W Med Ctr Dr,5200 MSRBIII, Ann Arbor, MI 48109 USA.
Dasgupta, Medhanjali (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Patwardhan, Anjali (författare)
Univ Michigan, Dept Biol Chem, Sch Med, 1150 W Med Ctr Dr,5200 MSRBIII, Ann Arbor, MI 48109 USA.
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Bogacz, Isabel (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Kaminsky, Corey (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Doyle, Margaret D. (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Chen, Percival Yang-Ting (författare)
MIT, Dept Chem, 77 Massachusetts Ave, Cambridge, MA 02139 USA.;Morph Therapeut, 35 Gatehouse Dr,A2, Waltham, MA 02451 USA.
Keable, Stephen M. (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Makita, Hiroki (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Simon, Philipp S. (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Massad, Ramzi (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.;Univ Calif Los Angeles, Dept Chem & Biochem, Los Angeles, CA 90095 USA.
Fransson, Thomas (författare)
KTH,Teoretisk kemi och biologi
Chatterjee, Ruchira (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Bhowmick, Asmit (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Paley, Daniel W. (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Moriarty, Nigel W. (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Brewster, Aaron S. (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Gee, Leland B. (författare)
SLAG Natl Accelerator Lab, LCLS, Menlo Pk, CA 94025 USA.
Alonso-Mori, Roberto (författare)
SLAG Natl Accelerator Lab, LCLS, Menlo Pk, CA 94025 USA.
Moss, Frank (författare)
SLAG Natl Accelerator Lab, LCLS, Menlo Pk, CA 94025 USA.
Fuller, Franklin D. (författare)
SLAG Natl Accelerator Lab, LCLS, Menlo Pk, CA 94025 USA.
Batyuk, Alexander (författare)
SLAG Natl Accelerator Lab, LCLS, Menlo Pk, CA 94025 USA.
Sauter, Nicholas K. (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Bergmann, Uwe (författare)
Univ Wisconsin, Dept Phys, Madison, WI 53706 USA.
Drennan, Catherine L. (författare)
MIT, Dept Chem, 77 Massachusetts Ave, Cambridge, MA 02139 USA.;MIT, Dept Biol, 77 Massachusetts Ave, Cambridge, MA 02139 USA.;MIT, Howard Hughes Med Inst, 77 Massachusetts Ave, Cambridge, MA 02139 USA.;Canadian Inst Adv Res, Bioinspired Solar Energy Program, Toronto, ON M5G 1M1, Canada.
Yachandra, Vittal K. (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Yano, Junko (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Kern, Jan F. (författare)
Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA.
Ragsdale, Stephen W. (författare)
Univ Michigan, Dept Biol Chem, Sch Med, 1150 W Med Ctr Dr,5200 MSRBIII, Ann Arbor, MI 48109 USA.
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Univ Michigan, Dept Biol Chem, Sch Med, 1150 W Med Ctr Dr,5200 MSRBIII, Ann Arbor, MI 48109 USA Lawrence Berkeley Natl Lab, Mol Biophys & Integrated Bioimaging Div, Berkeley, CA 94720 USA. (creator_code:org_t)
Elsevier BV, 2022
2022
Engelska.
Ingår i: Journal of Inorganic Biochemistry. - : Elsevier BV. - 0162-0134 .- 1873-3344. ; 230, s. 111768-
Relaterad länk:
https://urn.kb.se/re...
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https://doi.org/10.1...
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  • Tidskriftsartikel (refereegranskat)
Abstract Ämnesord
Stäng  
  • Methyl-Coenzyme M Reductase (MCR) catalyzes the biosynthesis of methane in methanogenic archaea, using a catalytic Ni-centered Cofactor F430 in its active site. It also catalyzes the reverse reaction, that is, the anaerobic activation and oxidation, including the cleavage of the C-H bond in methane. Because methanogenesis is the major source of methane on earth, understanding the reaction mechanism of this enzyme can have massive implications in global energy balances. While recent publications have proposed a radical-based catalytic mechanism as well as novel sulfonate-based binding modes of MCR for its native substrates, the structure of the active state of MCR, as well as a complete characterization of the reaction, remain elusive. Previous attempts to structurally characterize the active MCR-Ni(I) state have been unsuccessful due to oxidation of the redox- sensitive catalytic Ni center. Further, while many cryo structures of the inactive Ni(II)-enzyme in various substrates bound forms have been published, no room temperature structures have been reported, and the structure and mechanism of MCR under physiologically relevant conditions is not known. In this study, we report the first room temperature structure of the MCRred1-silent Ni(II) form using an X-ray Free-Electron Laser (XFEL), with simultaneous X-ray Emission Spectroscopy (XES) and X-ray Diffraction (XRD) data collection. In celebration of the seminal contributions of inorganic chemist Dick Holm to our understanding of nickel-based catalysis, we are honored to announce our findings in this special issue dedicated to this remarkable pioneer of bioinorganic chemistry.

Ämnesord

NATURVETENSKAP  -- Biologi -- Biokemi och molekylärbiologi (hsv//swe)
NATURAL SCIENCES  -- Biological Sciences -- Biochemistry and Molecular Biology (hsv//eng)
NATURVETENSKAP  -- Kemi -- Analytisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Analytical Chemistry (hsv//eng)

Nyckelord

Methanogens
Nickel
X-ray Free-Electron Laser (XFEL)
Serial femtosecond crystallography (SFX)
X-ray Diffraction (XRD)
X-ray Emission Spectroscopy (XES)

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