Cryo-annealing of Photoreduced CdS Quantum Dot–Nitrogenase MoFe Protein Complexes Reveals the Kinetic Stability of the E 4 (2N2H) Intermediate

Vansuch, Gregory E.; Mulder, David W.; Chica, Bryant; Ruzicka, Jesse L.; Yang, Zhi-Yong; Pellows, Lauren M.; Willis, Mark A.; Brown, Katherine A.; Seefeldt, Lance C.; Peters, John W.; Dukovic, Gordana; King, Paul W.

doi:10.1021/jacs.3c06832

Cryo-annealing of Photoreduced CdS Quantum Dot–Nitrogenase MoFe Protein Complexes Reveals the Kinetic Stability of the E ₄ (2N2H) Intermediate

Journal Article · Wed Sep 20 00:00:00 EDT 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c06832· OSTI ID:2001156

Vansuch, Gregory E. ^[1]; ^[1]; ^[1]; Ruzicka, Jesse L. ^[2]; ^[3]; ^[2]; Willis, Mark A. ^[4]; ^[1]; ^[3]; Peters, John W. ^[5]; ^[6]; ^[7]

Biosciences Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States
Department of Chemistry, University of Colorado Boulder, Boulder, Colorado 80309, United States
Department of Chemistry and Biochemistry, Utah State University, Logan, Utah 84322, United States
Institute of Biological Chemistry, Washington State University, Pullman, Washington 99163, United States
Institute of Biological Chemistry, Washington State University, Pullman, Washington 99163, United States, Department of Chemistry and Biochemistry, University of Oklahoma, Norman, Oklahoma 73019, United States
Department of Chemistry, University of Colorado Boulder, Boulder, Colorado 80309, United States, Materials Science and Engineering, University of Colorado Boulder, Boulder, Colorado 80303, United States, Renewable and Sustainable Energy Institute, University of Colorado Boulder, Boulder, Colorado 80303, United States
Biosciences Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States, Renewable and Sustainable Energy Institute, University of Colorado Boulder, Boulder, Colorado 80303, United States

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 2001156

Alternate ID(s):: OSTI ID: 2005557

Report Number(s):: NREL/JA--2700-87497

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 39 Vol. 145; ISSN 0002-7863

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (25)

Novel EPR signals associated with FeMoco centres of MoFe protein in MgADP‐inhibited turnover of nitrogenase Maritano, Silvana; Fairhurst, Shirley A.; Eady, Robert R. FEBS Letters, Vol. 505, Issue 1 https://doi.org/10.1016/S0014-5793(01)02800-9	journal	August 2001
Active intermediates in heme monooxygenase reactions as revealed by cryoreduction/annealing, EPR/ENDOR studies Davydov, Roman; Hoffman, Brian M. Archives of Biochemistry and Biophysics, Vol. 507, Issue 1 https://doi.org/10.1016/j.abb.2010.09.013	journal	March 2011
Control of electron transfer in nitrogenase Seefeldt, Lance C.; Peters, John W.; Beratan, David N. Current Opinion in Chemical Biology, Vol. 47 https://doi.org/10.1016/j.cbpa.2018.08.011	journal	December 2018
Mechanistic Insights into Nitrogenase FeMo-Cofactor Catalysis through a Steady-State Kinetic Model Harris, Derek F.; Badalyan, Artavazd; Seefeldt, Lance C. Biochemistry, Vol. 61, Issue 19 https://doi.org/10.1021/acs.biochem.2c00415	journal	September 2022
Reduction of Substrates by Nitrogenases Seefeldt, Lance C.; Yang, Zhi-Yong; Lukoyanov, Dmitriy A. Chemical Reviews, Vol. 120, Issue 12 https://doi.org/10.1021/acs.chemrev.9b00556	journal	March 2020
Hydride Conformers of the Nitrogenase FeMo-cofactor Two-Electron Reduced State E ₂ (2H), Assigned Using Cryogenic Intra Electron Paramagnetic Resonance Cavity Photolysis Lukoyanov, Dmitriy A.; Khadka, Nimesh; Yang, Zhi-Yong Inorganic Chemistry, Vol. 57, Issue 12 https://doi.org/10.1021/acs.inorgchem.8b00271	journal	March 2018
The Kinetics of Electron Transfer from CdS Nanorods to the MoFe Protein of Nitrogenase Ruzicka, Jesse L.; Pellows, Lauren M.; Kallas, Hayden The Journal of Physical Chemistry C, Vol. 126, Issue 19 https://doi.org/10.1021/acs.jpcc.2c02528	journal	May 2022
Excitation-Rate Determines Product Stoichiometry in Photochemical Ammonia Production by CdS Quantum Dot-Nitrogenase MoFe Protein Complexes Brown, Katherine A.; Ruzicka, Jesse; Kallas, Hayden ACS Catalysis, Vol. 10, Issue 19 https://doi.org/10.1021/acscatal.0c02933	journal	September 2020
Nitrogenase: A Draft Mechanism Hoffman, Brian M.; Lukoyanov, Dmitriy; Dean, Dennis R. Accounts of Chemical Research, Vol. 46, Issue 2 https://doi.org/10.1021/ar300267m	journal	December 2012
Electron Paramagnetic Resonance Analysis of Different Azotobacter vinelandii Nitrogenase MoFe-Protein Conformations Generated during Enzyme Turnover: Evidence for S = ³ / ₂ Spin States from Reduced MoFe-Protein Intermediates ^† Fisher, Karl; Newton, William E.; Lowe, David J. Biochemistry, Vol. 40, Issue 11 https://doi.org/10.1021/bi0012686	journal	March 2001
Trapping an Intermediate of Dinitrogen (N ₂ ) Reduction on Nitrogenase Barney, Brett M.; Lukoyanov, Dmitriy; Igarashi, Robert Y. Biochemistry, Vol. 48, Issue 38 https://doi.org/10.1021/bi901092z	journal	September 2009
Trapping H ^- Bound to the Nitrogenase FeMo-Cofactor Active Site during H ₂ Evolution: Characterization by ENDOR Spectroscopy Igarashi, Robert Y.; Laryukhin, Mikhail; Dos Santos, Patricia C. Journal of the American Chemical Society, Vol. 127, Issue 17 https://doi.org/10.1021/ja043596p	journal	May 2005
Defining Intermediates of Nitrogenase MoFe Protein during N ₂ Reduction under Photochemical Electron Delivery from CdS Quantum Dots Chica, Bryant; Ruzicka, Jesse; Kallas, Hayden Journal of the American Chemical Society, Vol. 142, Issue 33 https://doi.org/10.1021/jacs.0c06343	journal	July 2020
Dissecting Electronic-Structural Transitions in the Nitrogenase MoFe Protein P-Cluster during Reduction Chica, Bryant; Ruzicka, Jesse; Pellows, Lauren M. Journal of the American Chemical Society, Vol. 144, Issue 13 https://doi.org/10.1021/jacs.1c13311	journal	March 2022
The Fe Protein Cycle Associated with Nitrogenase Catalysis Requires the Hydrolysis of Two ATP for Each Single Electron Transfer Event Yang, Zhi-Yong; Badalyan, Artavazd; Hoffman, Brian M. Journal of the American Chemical Society, Vol. 145, Issue 10 https://doi.org/10.1021/jacs.2c09576	journal	March 2023
Identification of a Key Catalytic Intermediate Demonstrates That Nitrogenase Is Activated by the Reversible Exchange of N ₂ for H ₂ Lukoyanov, Dmitriy; Yang, Zhi-Yong; Khadka, Nimesh Journal of the American Chemical Society, Vol. 137, Issue 10 https://doi.org/10.1021/jacs.5b00103	journal	March 2015
Reductive Elimination of H ₂ Activates Nitrogenase to Reduce the N≡N Triple Bond: Characterization of the E ₄ (4H) Janus Intermediate in Wild-Type Enzyme Lukoyanov, Dmitriy; Khadka, Nimesh; Yang, Zhi-Yong Journal of the American Chemical Society, Vol. 138, Issue 33 https://doi.org/10.1021/jacs.6b06362	journal	August 2016
Crystallographic structure and functional implications of the nitrogenase molybdenum–iron protein from Azotobacter vinelandii Kirn, Jongsun; Rees, D. C. Nature, Vol. 360, Issue 6404 https://doi.org/10.1038/360553a0	journal	December 1992
The E3 state of FeMoco: one hydride, two hydrides or dihydrogen? Pang, Yunjie; Bjornsson, Ragnar Physical Chemistry Chemical Physics, Vol. 25, Issue 31 https://doi.org/10.1039/D3CP01106B	journal	January 2023
The mechanism of Klebsiella pneumoniae nitrogenase action. Pre-steady-state kinetics of H2 formation Lowe, D. J.; Thorneley, R. N. Biochemical Journal, Vol. 224, Issue 3 https://doi.org/10.1042/bj2240877	journal	December 1984
Connecting nitrogenase intermediates with the kinetic scheme for N2 reduction by a relaxation protocol and identification of the N2 binding state Lukoyanov, D.; Barney, B. M.; Dean, D. R. Proceedings of the National Academy of Sciences, Vol. 104, Issue 5 https://doi.org/10.1073/pnas.0610975104	journal	January 2007
Critical computational analysis illuminates the reductive-elimination mechanism that activates nitrogenase for N ₂ reduction Raugei, Simone; Seefeldt, Lance C.; Hoffman, Brian M. Proceedings of the National Academy of Sciences, Vol. 115, Issue 45 https://doi.org/10.1073/pnas.1810211115	journal	October 2018
Stretched exponential relaxation in molecular and electronic glasses Phillips, J. C. Reports on Progress in Physics, Vol. 59, Issue 9 https://doi.org/10.1088/0034-4885/59/9/003	journal	September 1996
A nitrogen pressure of 50 atmospheres does not prevent evolution of hydrogen by nitrogenase Simpson, F.; Burris, R. Science, Vol. 224, Issue 4653 https://doi.org/10.1126/science.6585956	journal	June 1984
Light-driven dinitrogen reduction catalyzed by a CdS:nitrogenase MoFe protein biohybrid Brown, K. A.; Harris, D. F.; Wilker, M. B. Science, Vol. 352, Issue 6284 https://doi.org/10.1126/science.aaf2091	journal	April 2016

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CdS
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catalytic mechanism
electron paramagnetic resonance spectroscopy
nanocrystal
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Cryo-annealing of Photoreduced CdS Quantum Dot–Nitrogenase MoFe Protein Complexes Reveals the Kinetic Stability of the E 4 (2N2H) Intermediate

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Cryo-annealing of Photoreduced CdS Quantum Dot–Nitrogenase MoFe Protein Complexes Reveals the Kinetic Stability of the E ₄ (2N2H) Intermediate