Aqueous Hydricity of Late Metal Catalysts as a Continuum Tuned by Ligands and the Medium

Journal of the American Chemical Society
Catherine L PitmanAlexander J M Miller

Abstract

Aqueous hydride transfer is a fundamental step in emerging alternative energy transformations such as H2 evolution and CO2 reduction. "Hydricity," the hydride donor ability of a species, is a key metric for understanding transition metal hydride reactivity, but comprehensive studies of aqueous hydricity are scarce. An extensive and self-consistent aqueous hydricity scale is constructed for a family of Ru and Ir hydrides that are key intermediates in aqueous catalysis. A reference hydricity is determined using redox potentiometry and spectrophotometric titration for a particularly water-soluble species. Then, relative hydricity values for a range of species are measured using hydride transfer equilibria, taking advantage of expedient new synthetic procedures for Ru and Ir hydrides. This large collection of hydricity values provides the most comprehensive picture so far of how ligands impact hydricity in water. Strikingly, we also find that hydricity can be viewed as a continuum in water: the free energy of hydride transfer changes with pH, buffer composition, and salts present in solution.

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Citations

Aug 3, 2016·Chemical Reviews·Eric S WiednerAaron M Appel
Sep 28, 2016·Journal of the American Chemical Society·Matthew B ChambersAlexander J M Miller
Oct 21, 2016·Journal of the American Chemical Society·Elisabetta AlbericoMatthias Beller
Mar 15, 2018·Chemical Communications : Chem Comm·F SchömbergI Vilotijevic
Mar 16, 2018·Chemical Society Reviews·Stefan IlicKsenija D Glusac
Mar 8, 2016·Chemical Communications : Chem Comm·C L PitmanA J M Miller
Jun 8, 2018·Chemistry : a European Journal·Eric S Wiedner, John C Linehan
Sep 30, 2017·Angewandte Chemie·Samantha A BurgessEric S Wiedner
Nov 23, 2018·Proceedings of the National Academy of Sciences of the United States of America·Bianca M Ceballos, Jenny Y Yang
Aug 12, 2020·Chemical Society Reviews·Kelsey R BreretonAlexander J M Miller
Jun 18, 2017·Chemical Communications : Chem Comm·Bianca M CeballosJenny Y Yang
Feb 13, 2019·Chemical Science·Xiaoxiao ChuWenguang Wang
Nov 26, 2020·Chemistry : a European Journal·Abhishek KumarJoyanta Choudhury
May 16, 2021·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Brian N DiMarcoEtsuko Fujita
Jun 15, 2021·Chemical Science·Mirjam R SchreierOliver S Wenger
Apr 20, 2018·The Journal of Physical Chemistry. a·Chelsea M TaliaferroFelix N Castellano
Dec 23, 2016·The Journal of Physical Chemistry. B·Kelsey R BreretonThomas R Cundari
Dec 10, 2016·Inorganic Chemistry·Kelsey R BreretonAlexander J M Miller
Mar 17, 2018·Journal of the American Chemical Society·Stefan IlicKsenija D Glusac
Apr 24, 2019·Journal of the American Chemical Society·Eric S Wiedner
Jun 24, 2020·The Journal of Physical Chemistry. a·Ashley S McNeillDavid A Dixon
Nov 4, 2020·Journal of the American Chemical Society·Jenny Y YangJeffrey M Barlow
Oct 20, 2021·Journal of the American Chemical Society·Francesca ArcudiEmily A Weiss
Dec 21, 2021·Chemical Reviews·Rishi G AgarwalJames M Mayer

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BETA
NMR

Software Mentioned

Aftermath
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