个人简介

American Chemical. Society Alfred Bader Award in Bioinorganic or Bioorganic Chemistry, 2008 Frontiers in Biological Chemistry Award from the Max-Planck-Institut für Bioanorganishe Chemie, 2005 Elected Fellow of the American Association for the Advancement of Science, 2001 National Institutes of Health MERIT Award 2000-2010 University of Minnesota Award for Outstanding Contributions in Post-Baccalaureate, Graduate, and Professional Education, 1999-2000 NIH Research Career Development Award, 1982-87 Alfred P. Sloan Research Fellowship, 1982-86

研究领域

Inorganic & Organometallic Chemistry/Chemical Biology/Environmental & Green Chemistry/Energy & Catalysis

Our group focuses on bio-inorganic chemistry, specifically on the topic of iron, oxygen and biocatalysis. Our research effort, involving a combination of biochemical, synthetic inorganic, and spectroscopic approaches, is aimed at elucidating the oxygen activation mechanisms of nonheme iron enzymes, designing functional models for such enzymes, trapping and characterizing reaction intermediates, and developing bio-inspired oxidation catalysts for green chemistry applications. The pictures illustrate a novel manganese dioxygenase we are investigating and the crystal structure of a recently isolated oxoiron(IV) complex.

近期论文

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Chiang, C.-W.; Kleespies, S. T.; Stout, H. D.; Meier, K. K.; Li, P.-Y.; Bominaar, E. L.; Que, L., Jr.; Münck, E.; Lee, W.-Z., Characterization of a Paramagnetic Mononuclear Nonheme Iron-Superoxo Complex. J. Am. Chem. Soc. 2014, 136, 10846–10849 (DOI: 10.1021/ja504410s; PMC4132977). Company, A.; Sabenya, G.; González-Béjar, M.; Gómez, L.; Clémancey, M.; Blondin, G.; Jasniewski, A. J.; Puri, M.; Browne, W. R.; Latour, J.-M.; Que, L., Jr.; Costas, M.; Pérez-Prieto, J.; Lloret-Fillol, J., Triggering the Generation of an Iron(IV)-Oxo Compound and Its Reactivity toward Sulfides by RuII Photocatalysis. J. Am. Chem. Soc. 2014, 136, 4624-4633 (DOI: 10.1021/ja412059c; PMC3985778 ). England, J.; Bigelow, J. O.; Heuvelen, K. M. V.; Farquhar, E. R.; Martinho, M.; Meier, K. K.; Frisch, J. R.; Münck, E.; Que, L., Jr., An Ultra-stable Oxoiron(IV) Complex and Its Blue Conjugate Base. Chem. Sci. 2014, 5, 1204-1215 (DOI: 10.1039/C3SC52755G; PMC 3956701). Fielding, A. J.; Lipscomb, J. D.; Que, L., Jr., A two-electron Shell Game: intermediates of the Extradiol Cleaving Catechol Dioxygenases. J. Biol. Inorg. Chem. 2014, 19, 491-504 (DOI:10.1007/s00775-014-1122-9; PMC4039383) . . Iyer, S. R.; Javadi, M. M.; Feng, Y.; Hyun, M. Y.; Oloo, W. N.; Kim, C.; Que, L., Jr., A Chameleon Catalyst forNnonheme Iron-promoted Olefin Oxidation. Chem. Commun. 2014, 50, 13777-13780 (DOI:10.1039/c4cc06164k; PMC In process). Makhlynets, O. V.; Oloo, W.; Moroza, Y. S.; Belayaa, I. G.; Palluccio, T. D.; Filatov, A. S.; Müller, P.; Cranswick, M. A.; Que, L., Jr.; Rybak-Akimova, E. V., H2O2 Activation with Biomimetic Non-haem Iron Complexes and AcOH: Connecting the g = 2.7 EPR Signal with a Visible Chromophore. Chem. Commun. 2014, 50, 645-648 (DOI: 10.1039/C1033CC47632D). Oloo, W.N.; Meier, K. K.; Wang, Y.; Shaik, S.; Münck, E.; Que, L., Jr., Identification of a Low-spin Acylperoxoiron(III) Intermediate in Bio-inspired Nonheme Iron-Catalyzed Oxidations. Nature Communications 2014, 5, 3046.(DOI: 10.1038/ncomms4046). Paine, T. K.; Que, L., Jr., Dioxygen Activation by Biomimetic Iron Complexes of α-Keto Acids and α-Hydroxy Acids. Struct. Bonding 2014, 160, 39-56. Stoian, S. A.; Xue, G.; Bominaar, E. L.; Que, L., Jr.; Münck, E., Spectroscopic and Theoretical Investigation of a Complex with a [O=FeIV–O–FeIV=O] Core Related to Methane Monooxygenase Intermediate Q. J. Am. Chem. Soc. 2014, 136, 1545-1558 (DOI: 10.1021/ja411376u; PMC3941033). Frisch, J. R.; McDonnell, R.; Rybak-Akimova, E. V.; Que, L., Jr., Factors Affecting the Carboxylate Shift Upon Formation of Nonheme Diiron-O2 Adducts. Inorg. Chem. 2013, 52, 2627-36 (10.1021/ic302543n; PMCID: PMC3678525 ). Hayden, J. A.; Farquhar, E. R.; Que, L., Jr.; Lipscomb, J. D.; Hendrich, M. P., NO Binding to Mn-Substituted Homoprotocatechuate 2,3-Dioxygenase and the Primary and Secondary Sphere Influences in O2 Reactivity. J. Biol. Inorg. Chem. 2013, 18, 717-728. (10.1007/s00775-013-1016-2; PMCID: PMC3936460). Li, F.; Van Heuvelen, K. M.; Meier, K. K.; Münck, E.; Que, L., Sc3+-triggered Oxoiron(IV) Formation from O2 and its Nonheme Iron(II) Precursor via a Sc3+-peroxo-Fe3+ Intermediate. J. Am. Chem. Soc. 2013, 135, 10198-10201 (10.1021/ja402645y; NSF). McDonald, A. R.; Que, L., Jr., High-Valent Nonheme Iron-Oxo Complexes: Synthesis, Structure, and Spectroscopy. Coord. Chem. Rev. 2013, 257, 414-428 (10.1016/j.ccr.2012.08.002). Oloo, W. N.; Feng, Y.; Iyer, S.; Parmelee, S.; Xue, G.; Que, L., Jr., Cyclohexene as a Substrate Probe for the Nature of the High-valent Iron-oxo Oxidant in Fe(TPA)-catalyzed Oxidations. New. J. Chem. 2013, 37, 3411-3415 (10.1039/C3NJ00524K; DOE). Oloo, W. N.; Fielding, A. J.; Que, L. J., Rate Determining Water-Assisted O–O Bond Cleavage of a FeIII–OOH Intermediate in a Bio-inspired Nonheme Iron-Catalyzed Oxidation. J. Am. Chem. Soc. 2013, 135, 6438 (doi: 10.1021/ja402759c). Oloo, W. N.; Que, L., Jr., "Hydrocarbon Oxidations Catalyzed by Bio-Inspired Nonheme Iron and Copper Catalysts.” In Comprehensive Inorganic Chemistry II; Reedijk, J., Poeppelmeier, K., Eds.; Elsevier: Oxford, 2013; Vol. 6, pp 763-778. Pap, J. S.; Cranswick, M. A.; Balogh-Hergovich, É.; Baráth, G.; Giorgi, M.; Rohde, G. T.; Kaizer, J.; Speier, G.; Que, L., Jr., An Iron(II)[1,3-bis(2?-pyridylimino)isoindoline] Complex as a Catalyst for Substrate Oxidation with H2O2- Evidence for a Transient Peroxidodiiron(III) Species. Eur. J. Inorg. Chem. 2013, 3858-3866 (10.1002/ejic.201300162,;PMCID: PMC3935335). Park, K.; Bell, C. B., 3rd; Liu, L. V.; Wang, D.; Xue, G.; Kwak, Y.; Wong, S. D.; Light, K. M.; Zhao, J.; Alp, E. E.; Yoda, Y.; Saito, M.; Kobayashi, Y.; Ohta, T.; Seto, M.; Que, L., Jr.; Solomon, E. I., Nuclear Resonance Vibrational Spectroscopic and Computational Study of High-valent Diiron Complexes Relevant to Enzyme Intermediates. Proc. Nat. Acad. Sci. USA 2013, 110, 6275 (doi: 10.1073/pnas.1304238110; PMC3631696). Prat, I.; Company, A.; Postils, V.; Ribas, X.; Que, L., Jr.; Luis, J. M.; Costas, M., The Mechanism of Stereospecific C–H Oxidation by Fe(Pytacn) Complexes: Bioinspired Non-Heme Iron Catalysts Containing cis-Labile Exchangeable Sites. Chem. Eur. J. 2013, 19, 6724 (doi: 10.1002/chem.201300110). Que, L., Jr., High-Valent Nonheme Iron Oxidants in Biology: Lessons from Synthetic FeIV=O Complexes. Bull. Jpn. Soc. Coord. Chem. 2013, 62, 30-37.