Szymczak, Nathaniel - University of Michigan

个人简介

Nathaniel (Nate) Szymczak was born in Wollongong, Australia. In 2002 he received his Bachelor of Science degree in chemistry (with a specialization in environmental chemistry) from the University of Illinois at Champaign-Urbana, where he was fortunate to work on several undergraduate research projects, each focused on a unique approach to environmentally-motivated chemistry. His research experience culminated in the laboratories of Professor Thomas Rauchfuss where he worked on synthetic bioinorganic chemistry. In the fall of 2002, Nate began doctoral studies under the direction of David Tyler at the University of Oregon. His graduate research focused on water-soluble transition metal dihydrogen and dinitrogen complexes as well as hydrogen-bonding interactions of a coordinated H2 ligand. As part of an NSF-IGERT graduate fellowship, he participated in a brief internship at the Pacific Northwest National Laboratory and worked with Dr. John Linehan to uncover the mechanism of hydrogen release from hydrogen storage materials, as well as to elucidate the active catalyst structure using Operando XAS methods. He was awarded a Ph.D. in 2007, and following doctoral studies, he pursued postdoctoral research with Professor Jonas Peters at the Massachusetts Institute of Technology and the California Institute of Technology. His work focused on the development of bimetallic macrocyclic coordination complexes for electrocatalytic proton reduction and other multi-electron transformations, as well as the development of reliable methods to electrochemically investigate homogeneous systems at elevated pressures. In 2010, Nate joined the faculty at the University of Michigan where his research program focuses primarily on synthetic transition-metal based inorganic chemistry targeted toward the development of new catalytic transformations for energy recycling and delivery with minimal energy input.

研究领域

Our research program uses fundamental principles of molecular design to address some of the grand challenges in the fields of small molecule activation and catalysis. We are interested in developing strategies to reversibly store energy in the form of chemical bonds, and also to rapidly convert abundant chemical (bio)feedstocks into value-added chemicals and fuels. The overarching themes of our research program are to (a) understand how to exploit carefully positioned secondary-sphere sites to control reactivity, and (b) develop transition metal compounds to promote otherwise difficult transformations of small molecule chemical feedstocks such as N2, CO2, O2, and CO. We are working to establish new ways by which molecular catalysts can be tuned by the incorporation of pendent functional groups within a metal’s secondary coordination sphere environment. We are using these appended functional groups (hydrogen bond donor/acceptors, or Lewis acid/bases) to augment reactivity of the central transition metal in order to promote the activation/delivery of small molecules to appropriate substrates. Overall, our approach aims to move the emphasis away from the transition metal, and instead, place high importance on secondary-coordination sphere interactions (not directly bound to the metal) to develop new metal complexes and catalysts that synergistically engage substrates for binding/reduction, regulate activity, and ultimately incorporate earth-abundant metals.

近期论文

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Dahl, E. W.; Kiernicki, J. J.; Zeller, M.; Szymczak, N. K.; Hydrogen Bonds Dictate O2 Capture and Release within a Zinc Tripod J. Am. Chem. Soc. 2018, DOI: 10.1021/jacs.8b04266 Geri, J. B.; Wade Wolfe, M. M.; Szymczak, N. K.; The Difluoromethyl Group as a Masked Nucleophile: A Lewis Acid/Base Approach J. Am. Chem. Soc. 2018, DOI: 10.1021/jacs.8b06093 Geri, J. B.; Ciatti, J. L.; Szymczak, N. K.; Charge effects regulate reversible CO2 reduction catalysis Chem. Commun. 2018, 54, 7790-7793. DOI: 10.1039/C8CC04370A Hale, L. V. A.; Szymczak, N. K.; Hydrogen Transfer Catalysis beyond the Primary Coordination Sphere ACS Catal. 2018, 8, 6446–6461. DOI: 10.1021/acscatal.7b04216 Dahl, E. W.; Dong, H. T.; Szymczak, N. K.; Phenylamino derivatives of tris(2-pyridylmethyl)amine: hydrogen-bonded peroxodicopper complexes Chem. Commun. 2018, 892-895 DOI: 10.1039/C7CC08619A Kiernicki, J. J.; Zeller, M.; Szymczak, N. K.; Hydrazine Capture and N–N Bond Cleavage at Iron Enabled by Flexible Appended Lewis Acids J. Am. Chem. Soc. 2017, 139, 18194–18197 DOI: 10.1021/jacs.7b11465 Geri, J. B.; Wade Wolfe, M. M.; Szymczak, N. K.; Borazine-CF3- Adducts for Rapid, Room Temperature, and Broad Scope Trifluoromethylation Angew. Chem. Int. Ed. 2018, 1381-1385 DOI: 10.1002/anie.201711316 Geri, J. B.; Szymczak, N. K.; Recyclable Trifluoromethylation Reagents from Fluoroform J. Am. Chem. Soc. 2017, 139, 9811-9814. DOI: 10.1021/jacs.7b05408 Geri, J. B.; Shanahan, J. P.; Szymczak, N. K.; Testing the Push–Pull Hypothesis: Lewis Acid Augmented N2 Activation at Iron J. Am. Chem. Soc. 2017, 139, 5952–5956. DOI: 10.1021/jacs.7b01982 Dahl, E. W.; Louis-Goff, T.; Szymczak, N. K.; Second sphere ligand modifications enable a recyclable catalyst for oxidant-free alcohol oxidation to carboxylates Chem. Commun. 2017, 53, 2287-2289. DOI: 10.1039/C6CC10206A Hale, L. V. A.; Szymczak, N. K.; Stereoretentive Deuteration of α-Chiral Amines with D2O J. Am. Chem. Soc. 2016, 138, 13489-13492. DOI: 10.1021/jacs.6b07879 Tseng, K. T.; Kampf, J. W.; Szymczak, N. K.; Modular Attachment of Appended Boron Lewis Acids to a Ruthenium Pincer Catalyst: Metal–Ligand Cooperativity Enables Selective Alkyne Hydrogenation J. Am. Chem. Soc. 2016, 138, 10378–10381. DOI: 10.1021/jacs.6b03972. Hale, L. V. A.; Malakar, T.; Tseng, K. T.; Zimmerman, P. M.; Paul, A.; Szymczak, N. K.; The Mechanism of Acceptorless Amine Double Dehydrogenation by N,N,N-Amide Ruthenium(II) Hydrides: A Combined Experimental and Computational Study ACS Catal. 2016, 6, 4799-4813. DOI: 10.1021/acscatal.6b01465. Moore, C. M.; Bark, B. Szymczak, N. K.; Simple Ligand Modifications with Pendent OH Groups Dramatically Impact the Activity and Selectivity of Ruthenium Catalysts for Transfer Hydrogenation: The Importance of Alkali Metals. ACS Catal. 2016, 6, 1981-1990. DOI: 10.1021/acscatal.6b00229. Dahl, E. W.; Szymczak, N. K.; Hydrogen Bonds Dictate the Coordination Geometry of Copper: Characterization of a Square-Planar Copper(I) Complex. Angew. Chem. Int. Ed. 2016, 55, 3101 –3105. DOI: 10.1002/anie.201511527. Tseng, K. T.; Lin, S.; Kampf, J. W.; Szymczak, N. K.; Upgrading Ethanol to 1-Butanol with a Homogeneous Air-Stable Ruthenium Catalyst. Chem. Commun. 2016, 52, 2901-2904. DOI: 10.1039/C5CC09913G. Geri, J. B.; Szymczak, N. K.; A Proton-Switchable Bifunctional Ruthenium Complex That Catalyzes Nitrile Hydroboration. J. Am. Chem. Soc. 2015, 137, 12808-12814. Carter, T. J.; Heiden, Z. M.; Szymczak, N. K.; Discovery of Low Energy Pathways to Metal Mediated B=N Bond Reduction Guided by Computation and Experiment. Chem. Sci. 2015, 6, 7258-7266. Tseng, K. T.; Kampf, J. W.; Szymczak, N. K.; Mechanism of N,N,N,-Amide Ruthenium(II) Hydride Mediated Acceptorless Alcohol Dehydrogenation: Inner-Sphere b-H Elimination versus Outer-Sphere Bufunctional Metal-Ligand Cooperativity. ACS Catal. 2015, 5, 5468-5485. Moore, C. M.; Szymczak, N. K.; Nitrite reduction by copper through ligand-mediated proton and electron transfer. Chem. Sci. 2015, 6, 3373-3377.