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Title: Thermodynamic Hydricity of Transition Metal Hydrides

Abstract

Transition metal hydrides play a critical role in stoichiometric and catalytic transformations. Knowledge of free energies for cleaving metal hydride bonds can enable the prediction of chemical reactivity, such as for the bond-forming and bond-breaking events that occur in a catalytic reaction. Thermodynamic hydricity is the free energy required to cleave an M–H bond to generate a hydride ion (H–). Three primary methods have been developed for hydricity determination: the “reference hydride” method establishes hydride transfer equilibrium with a hydride donor/acceptor pair of known hydricity, the “H2 heterolysis” method involves measuring the equilibrium of heterolytic cleavage of H2 in the presence of a base, and the “potential–pKa” method considers stepwise transfer of a proton and two electrons to give a net hydride transfer. Using these methods, over 100 thermodynamic hydricity values for transition metal hydrides have been determined in acetonitrile or water. In acetonitrile, the hydricity of metal hydrides spans a range of more than 50 kcal/mol. Methods for using hydricity values to predict chemical reactivity are also discussed, including organic transformations, the reduction of CO2, and the production and oxidation of hydrogen. E.S.W. and A.M.A. were supported by the U.S. Department of Energy, Office of Science, Office of Basicmore » Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. R.M.B. was supported by the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy. M.B.C. and A.J.M.M. were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences (DE-SC0014255). C.L.P. was supported by the National Science Foundation Center for Enabling New Technologies through Catalysis (CHE-1205189) and the Royster Society of Fellows (C.L.P.).« less

Authors:
 [1];  [2];  [2];  [1];  [2];  [1]
+ Show Author Affiliations
  1. Pacific Northwest National Laboratory, Richland, Washington 99352, United States
  2. Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599-3290, United States
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Molecular Electrocatalysis (CME)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1280195
Alternate Identifier(s):
OSTI ID: 1313998; OSTI ID: 1773427
Report Number(s):
PNNL-SA-116484
Journal ID: ISSN 0009-2665
Grant/Contract Number:  
SC0014255; CHE-1205189; AC05-76RL01830
Resource Type:
Published Article
Journal Name:
Chemical Reviews
Additional Journal Information:
Journal Name: Chemical Reviews Journal Volume: 116 Journal Issue: 15; Journal ID: ISSN 0009-2665
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; hydride; hydricity; catalysis; hydrogen; carbon dioxide

Citation Formats

Wiedner, Eric S., Chambers, Matthew B., Pitman, Catherine L., Bullock, R. Morris, Miller, Alexander J. M., and Appel, Aaron M.. Thermodynamic Hydricity of Transition Metal Hydrides. United States: N. p., 2016. Web. doi:10.1021/acs.chemrev.6b00168.
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Wiedner, Eric S., Chambers, Matthew B., Pitman, Catherine L., Bullock, R. Morris, Miller, Alexander J. M., & Appel, Aaron M.. Thermodynamic Hydricity of Transition Metal Hydrides. United States. https://doi.org/10.1021/acs.chemrev.6b00168
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Wiedner, Eric S., Chambers, Matthew B., Pitman, Catherine L., Bullock, R. Morris, Miller, Alexander J. M., and Appel, Aaron M.. Tue . "Thermodynamic Hydricity of Transition Metal Hydrides". United States. https://doi.org/10.1021/acs.chemrev.6b00168.
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@article{osti_1280195,
title = {Thermodynamic Hydricity of Transition Metal Hydrides},
author = {Wiedner, Eric S. and Chambers, Matthew B. and Pitman, Catherine L. and Bullock, R. Morris and Miller, Alexander J. M. and Appel, Aaron M.},
abstractNote = {Transition metal hydrides play a critical role in stoichiometric and catalytic transformations. Knowledge of free energies for cleaving metal hydride bonds can enable the prediction of chemical reactivity, such as for the bond-forming and bond-breaking events that occur in a catalytic reaction. Thermodynamic hydricity is the free energy required to cleave an M–H bond to generate a hydride ion (H–). Three primary methods have been developed for hydricity determination: the “reference hydride” method establishes hydride transfer equilibrium with a hydride donor/acceptor pair of known hydricity, the “H2 heterolysis” method involves measuring the equilibrium of heterolytic cleavage of H2 in the presence of a base, and the “potential–pKa” method considers stepwise transfer of a proton and two electrons to give a net hydride transfer. Using these methods, over 100 thermodynamic hydricity values for transition metal hydrides have been determined in acetonitrile or water. In acetonitrile, the hydricity of metal hydrides spans a range of more than 50 kcal/mol. Methods for using hydricity values to predict chemical reactivity are also discussed, including organic transformations, the reduction of CO2, and the production and oxidation of hydrogen. E.S.W. and A.M.A. were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences. R.M.B. was supported by the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for the U.S. Department of Energy. M.B.C. and A.J.M.M. were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences (DE-SC0014255). C.L.P. was supported by the National Science Foundation Center for Enabling New Technologies through Catalysis (CHE-1205189) and the Royster Society of Fellows (C.L.P.).},
doi = {10.1021/acs.chemrev.6b00168},
journal = {Chemical Reviews},
number = 15,
volume = 116,
place = {United States},
year = {2016},
month = {8}
}
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  • Organometallics, Vol. 3, Issue 4
  • DOI: 10.1021/om00082a030

Thermodynamics of the Metal–Hydrogen Bonds in (η 5 -C 5 H 5 )M(CO) 2 H (M = Fe, Ru, Os)
journal, June 2011

  • Estes, Deven P.; Vannucci, Aaron K.; Hall, Ariel R.
  • Organometallics, Vol. 30, Issue 12
  • DOI: 10.1021/om2001519

Relative rates of hydrogen atom (H.cntdot.) transfer from transition-metal hydrides to trityl radicals
journal, June 1991

  • Eisenberg, David C.; Lawrie, Christophe J. C.; Moody, Anne E.
  • Journal of the American Chemical Society, Vol. 113, Issue 13
  • DOI: 10.1021/ja00013a026

Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO 2 Fixation
journal, June 2013

  • Appel, Aaron M.; Bercaw, John E.; Bocarsly, Andrew B.
  • Chemical Reviews, Vol. 113, Issue 8
  • DOI: 10.1021/cr300463y

Fuel from Water: The Photochemical Generation of Hydrogen from Water
journal, June 2014

  • Han, Zhiji; Eisenberg, Richard
  • Accounts of Chemical Research, Vol. 47, Issue 8
  • DOI: 10.1021/ar5001605

Ab Initio Calculations of p K a Values of Transition-Metal Hydrides in Acetonitrile
journal, December 2006

  • Qi, Xiu-Juan; Liu, Lei; Fu, Yao
  • Organometallics, Vol. 25, Issue 25
  • DOI: 10.1021/om0608859

A Thermodynamic Analysis of Rhenium(I)–Formyl C–H Bond Formation via Base-Assisted Heterolytic H 2 Cleavage in the Secondary Coordination Sphere
journal, September 2013

  • Teets, Thomas S.; Labinger, Jay A.; Bercaw, John E.
  • Organometallics, Vol. 32, Issue 19
  • DOI: 10.1021/om400810v

Acid−Base Equilibria in Nonpolar Media. 1. A Spectrophotometric Method for Acidity Measurements in Heptane
journal, November 1997

  • Leito, Ivo; Rodima, Toomas; Koppel, Ilmar A.
  • The Journal of Organic Chemistry, Vol. 62, Issue 24
  • DOI: 10.1021/jo9713013

Water-Soluble Phenanthroline Complexes of Rhodium, Iridium and Ruthenium for the Regeneration of NADH in the Enzymatic Reduction of Ketones
journal, October 2007

  • Canivet, Jérôme; Süss-Fink, Georg; Štěpnička, Petr
  • European Journal of Inorganic Chemistry, Vol. 2007, Issue 30
  • DOI: 10.1002/ejic.200700505
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