个人简介

Ph.D., Stanford University

研究领域

Chemical catalysis/nanoparticle research/energy research and kinetics and mechanism

Heterogeneous Artificial Photosynthesis Systems for Complete Fuel Forming Reactions: Harnessing solar energy is necessary for creating a sustainable energy future. We are currently developing artificial photosynthetic systems capable of complete fuel forming reactions, including water splitting. This project is in collaboration with Brian Gregg of the National Renewable Energy Laboratories in Golden, CO. Water Oxidation Catalysis: Who’s the Catalyst? The oxidation of water coupled to proton or CO2 reduction is necessary for fuel forming reactions; vide supra. Water oxidation is currently the kinetic bottle neck of this reaction when H2 is generated as the fuel. In water oxidation catalysis (WOC), as with all catalysis, the identity of the true catalyst must be known in order to optimize and rationally synthesize the next generation of catalysts. We have demonstrated, along with others, that many claimed WOC’s are actually catalytic precursors to highly active heterogeneous catalysts. We are currently working with the best known catalysts to answer the question “who’s the catalyst?” en route to long-lived and highly active WOC’s. Kinetic and Mechanistic Studies of Nanoparticle Formation and Catalysis: Starting from a well-defined Ir(1,5-COD)P2W15Nb3O62 precursor, we have unraveled what looks to be a much more widely applicable mechanism governing the self-assembly of transition metal nanoparticles. In addition, we now understand their stabilization mechanisms and catalysis. Currently, we are extending our kinetic and mechanistic studies to the formation of supported-nanoparticle heterogeneous catalyst formation in contact with solution—en route to improved heterogeneous catalysts; the most industrially important types of catalysts. Understanding Nucleation and Growth Across Nature: Our kinetic and mechanistic studies of nanocluster formation led to the development of a 2-step mechanism of nucleation (A ➝ B, k1) and growth (A + B ➝ 2B, k2). We are currently exploring its relation to a broader range of self assembly systems across nature including: (i) supported-nanoparticle heterogeneous catalyst formation, (ii) proteins in neurological diseases, (iii) solid-state phase transformations﹣including Avrami type transformations, (iv) organometallic catalyst formation and (v) dioxygenase oxidation catalysis. This is a wide-open area that involves everything from kinetic studies, computational work, XAFS and other synchrotron-radiation methods, plus the analysis of diverse areas of scientific literature.

近期论文

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The Tri-Niobium, Wells-Dawson Type Polyoxoanion, [(n C4H9)4N]9P2W15Nb3O62: Improvements in the Synthesis, Its Reliability, the Purity of the Product and the Detailed Synthetic Procedure. Laxson, W. W.; Özkar, S.; Finke, R. G., Inorg. Chem., 2014, 53, 2666-2676. Visible-light assisted photoelectrochemical water oxidation by thin films of a phosphonate-functionalized perylene diimide plus CoOx cocatalyst. Kirner, J. T.; Stracke, J. J.; Gregg , B. A.; Finke, R. G., ACS Applied Materials & Interfaces, 2014, 6, 13367-13377 ("ACS Editors’ Choice Article Selection"; selected as Cover Art; also most read distinction). Distinguishing Homogeneous from Heterogeneous Water Oxidation Catalysis When Beginning with Polyoxometalates. Stracke, J. J.; Finke, R. G. ACS Catalysis, 2014, 4, 909-933. A Four-Step Mechanism for the Formation of Supported-Nanoparticle Heterogeneous Catalysts in Contact with Solution: The Conversion of Ir(1,5-COD)Cl/γ-Al2O3 to Ir(0)~170/γ-Al2O3. Kent, P. D.; Mondloch, J. E.; Finke, R. G. J. Am. Chem. Soc. 2014, 136, 1930-1941. Water Oxidation Catalysis Beginning with Co4(H2O)2(PW9O34)10- when Driven by the Chemical Oxidant Ruthenium(III)tris(2,2’-bipyridine): Stoichiometry, Kinetic, and Mechanistic Studies En Route to Identifying the True Catalyst. Stracke, J. J.; Finke, R. G. ACS Catalysis, 2014, 4, 79-89. Water oxidation catalysis beginning with 2.5 µM [Co4(H2O)2(PW9O34)2]10-: Investigation of the true electrochemically driven catalyst at ≥600 mV overpotential at a glassy carbon electrode:, Stracke, J. J.; Finke, R. G. ACS Catalysis, 2013, 3, 1209-1219. Exceptionally Thermally Stable, Hydrocarbon Soluble Ziegler-type Ir(0)n Nanoparticle Catalysts Made from [Ir(1,5-COD)(µ-O2C8H15)]2 Plus AlEt3: Tests of Key Hypotheses for Their Unusual Stabilization. Hamdemir, I. K.; Özkar, S.; Finke, R. G, J. Mol. Catal. A, 2013, 378, 333-343. A Review of the Kinetics and Mechanisms of Formation of Supported-Nanoparticle Heterogeneous Catalysts. Mondloch, J. E.; Bayram, E.; Finke, J. Mol. Catal. A, 2012, 355, 1-38. ("Editor’s Choice" selection). Gold Nanocluster Agglomeration Kinetic Studies: Evidence for Parallel Bimolecular Plus Autocatalytic Agglomeration Pathways as a Mechanistic Alternative to an Avrami-Based Analysis. Shields, S., Buhro, W. E., Finney, E. E.; Finke, R. G., Chemistry of Materials, 2012, 24, 1718-1725. Synthesis and Characterization of [(1,5-Cyclooctadiene)Ir(µ-H)]4: A Multipurpose, Tetrametallic, Coordinatively Unsaturated Ir4-Based Precatalyst and Synthon. Yih, K.-H.; Hamdemir, Isil K.; Mondloch, J. M.; Bayram, E.; Özkar, S.; Vasic, R.; Frenkel A. I.; Anderson, O.; Finke, R. G. Inorganic Chemistry, 2012, 51, 3186-3193. Kinetic Evidence for Bimolecular Nucleation In Supported-Transition-Metal-Nanoparticle Catalyst Formation In Contact With Solution: The Prototype Ir(1,5-COD)Cl/γ-Al2O3 to Ir(0)~900/γ-Al2O3 System. Mondloch, J. E.; Bayram, E.; Finke, R. G. ACS Catalysis, 2012, 2, 298-305. Hydrocarbon-Soluble, Isolable Ziegler-type Ir(0)n Nanoparticle Catalysts Made from [(1,5-COD)Ir(µ-O2C8H15)]2 and 2-5 Equivalents of AlEt3: Their High Catalytic Activity, Long Lifetime and AlEt3-Dependent, Exceptional, 200 °C Thermal Stability. Hamdemir, I. K.; Özkar, S.; Yih, K. H.; Mondloch, J. M.; Finke, R. G., ACS Catalysis, 2012, 2, 632-641. Quantitative 1,10-Phenanthroline Catalyst-Poisoning Kinetic Studies of Rh(0)n Nanoparticle and Rh4 Cluster Benzene Hydrogenation Catalysts: Estimates of the Poison Kassociation Binding Constants, of the Equivalents of Poison Bound and of the Number of Catalytically Active Sites for Each Catalyst. Bayram, E.; Finke, R. G. ACS Catalysis, 2012, 2, 1967-1975. Mononuclear Zeolite-Supported Iridium: Kinetic, Spectroscopic, Electron Microscopic, and Size-Selective Poisoning Evidence for an Atomically Dispersed True Catalyst at 22 o°C. Bayram, E.; Lu, J.; Aydin, C.; Uzun, A.; Browning, N. D.; Gates, B. C.; Finke, R. G. ACS Catalysis, 2012, 2, 1947-1957. Supported-Nanoparticle Heterogeneous Catalyst Formation in Contact with Solution: Kinetics and Mechanism of the Conversion of Ir(1,5-COD)Cl/γ-Al2O3 to Ir(0)~900/γ-Al2O3. Mondloch, J. E.; Finke, R. G. J. Am. Chem. Soc, 2011, 133, 7744-7756. Industrial Ziegler-type Hydrogenation Catalysts made from Co(neodecanoate)2 or Ni(2-ethylhexanoate)2, and AlEt3: Evidence for Nanoclusters and Sub-Nanocluster or Larger Ziegler-Nanocluster Based Catalysis, Alley, W. M.; Hamdemir, I. K.; Wang, Q.; Frenkel, A.; Li, L.; Yang, J. C.; Menard, L. D.; Nuzzo, R. G.; Özkar, S.; Yih, K. H.; Johnson, K.; Finke, R. G. Langmuir, 2011, 27, 6279-6294. Improved Syntheses for the Compounds [(1,5-COD)M(μ-O2C8H15)]2 (M is Ir or Rh). Alley, W. M.; Yih, K. H.; Finke, R. G. Organometallics, 2011, 30, 5068-5070. Electrocatalytic water oxidation beginning with the cobalt polyoxometalate [Co4(H2O)2(PW9O34)2]10-: Identification of heterogeneous CoOx as the dominant catalyst. Stracke, J. J.; Finke, R. G. J. Am. Chem. Soc, 2011, 133, 14872-14875. Is It Homogeneous or Heterogeneous Catalysis Derived from [RhCp*Cl2]2? In Operando XAFS, Kinetic and Crucial Kinetic Poisoning Evidence for Subnanometer Rh4 Cluster-Based Benzene Hydrogenation Catalysis. Bayram, E.; Linehan, J. C.; Fulton, J. L.; Roberts, J. A.S.; Szymczak, N. K.; Smurthwaite, T. D.; Özkar, S.; Balasubramanian, M.; Finke, R. G., J. Am. Chem. Soc, 2011, 133, 18889-18902. Reply to the Comment on "Fitting and Interpreting Transition-Metal Nanocluster Formation and Other Sigmoidal-Appearing Kinetic Data: A More Thorough Testing of Dispersive Kinetic vs Chemical-Mechanism-Based Equations and Treatments for 4-Step Type Kinetic Data", Finney, E. E.; Finke, R. G. Chem. Mater. 2010, 22, 2687-2688. Stereospecific Polymerization of Chiral Oxazolidinone-Functionalized Alkenes. Miyake, G. M.; DiRocco, D. A.; Liu, Q.; Oberg, K. M.; Bayram, E.; Finke, R. G.; Rovis, T.; Chen. E. Y.-X. Macromolecules 2010, 43, 7504-7514. Iridium Ziegler-Type Hydrogenation Catalysts Made from [(1,5-COD)Ir(μ-O2C8H15)]2 and AlEt3: Spectroscopic and Kinetic Evidence for the Irn Species Present and for Nanoparticles as the Fastest Catalyst. Alley, W. M.; Hamdemir, I. K.; Wang, Q.; Frenkel, A. I.; Li, L.; Yang, J. C.; Menard, L. D.; Nuzzo, R. G.; Ozkar, S.; Johnson, K. A.; Finke, R. G. Inorg. Chem. 2010, 49, 8131-8147. Development Plus Kinetic and Mechanistic Studies of a Prototype Supported-Nanoparticle Heterogeneous Catalyst Formation System in Contact with Solution: Ir(1,5-COD)Cl/γ-Al2O3 and Its Reduction by H2 to Ir(0)n/γ-Al2O3. Mondloch, J. E.; Finke, R. G. Journal of the American Chemical Society 2010, 132, 9701-9714. In Situ Formed "Weakly Ligated/Labile Ligand" Iridium(0) Nanoparticles and Aggregates as Catalysts for the Complete Hydrogenation of Neat Benzene at Room Temperature and Mild Pressures. Bayram, E.; Zahmakiran, M.; Ozkar, S.; Finke, R. G. Langmuir 2010, 26(14), 12455-12464. Ziegler-Type Hydrogenation Catalysts Made from Group 8-10 Transition Metal Precatalysts and AlR3 Cocatalysts: A critical Review of the Literature. Alley, W. M.; Hamdemir, I. K.; Johnson, K. A.; Finke, R. G. J. Mol. Catal. A-Chemical 2010, 315, (1), 1-27. Model Ziegler-Type Hydrogenation Catalyst Precursors, [(1,5-COD)M(μ-O2C8H15)]2 (M = Ir and Rh): Synthesis, Characterization, and Demonstration of Catalytic Activity En Route to Identifying the True Industrial Hydrogenation Catalysts. Alley, W. M.; Girard, C. W.; Ozkar, S.; Finke, R. G. Inorg. Chem. 2009; 48, (3), 1114-1121. Fitting and Interpreting Transition-Metal Nanocluster Formation and Other Sigmoidal-Appearing Kinetic Data: A More Thorough Testing of Dispersive Kinetic vs Chemical-Mechanism-Based Equations and Treatments for 4-Step Type Kinetic Data. Finney, E. E.; Finke, R. G. Chemistry of Materials 2009, 21 (19), 4468-4479. Also see: Reply to Comment on "Fitting and Interpreting Transition-Metal Nanocluster Formation and Other Sigmoidal-Appearing Kinetic Data: A More Thorough Testing of Dispersive Kinetic vs Chemical-Mechanism-Based Equations and Treatments for 4-Step Type Kinetic Data" Finney, E. E.; Finke, R. G. Chemistry of Materials, 2010, 22, 2687-2688. Is There a Minimal Chemical Mechanism Underlying Classical Avrami-Erofe’ev Treatments of Phase-Transformation Kinetic Data? Finney, E. E.; Finke, R. G. Chemistry of Materials 2009, 21 (19), 4692-4705. Ranking the Lacunary (Bu4N)9{H(alpha(2)-P2W17O61} Polyoxometalate’s Stabilizing Ability for Ir(0)n Nanocluster Formation and Stabilization Using the Five-Criteria Method Plus Necessary Control Experiments. Graham, C. R.; Ott, L. S.; Finke, R. G. Langmuir 2009, 25 (3), 1327-1336.