Distinct Bimetallic Cooperativity Among Water Reduction Catalysts Containing [CoIIICoIII], [NiIINiII], and [ZnIIZnII] Cores

Morgan, Fredricka; Schaugaard, Richard; Anderson, Dennis; Schlegel, H. Bernhard; Verani, Cláudio N.

doi:10.1002/chem.202104426

Title: Distinct Bimetallic Cooperativity Among Water Reduction Catalysts Containing [Co^IIICo^III], [Ni^IINi^II], and [Zn^IIZn^II] Cores

Journal Article · 25 February 2022 · Chemistry - A European Journal

DOI: https://doi.org/10.1002/chem.202104426 · OSTI ID:1976300

Morgan, Fredricka ^[1];

^[1]; Anderson, Dennis ^[1];

^[1];

^[1]

Wayne State University, Detroit, MI (United States)

Abstract Three binuclear species [LCo ^III ₂ (μ‐Pz) ₂ ](ClO ₄ ) ₃ ( 1 ), [LNi ^II ₂ (CH ₃ OH) ₂ Cl ₂ ]ClO ₄ ( 2 ), and [LZn ^II ₂ Cl ₂ ]PF ₆ ( 3 ) supported by the deprotonated form of the ligand 2,6‐bis[bis(2‐pyridylmethyl) amino‐methyl]‐4‐methylphenol were synthesized, structurally characterized as solids and in solution, and had their electrochemical and spectroscopic behavior established. Species 1 – 3 had their water reduction ability studied aiming to interrogate the possible cooperative catalytic activity between two neighboring metal centers. Species 1 and 2 reduced H ₂ O to H ₂ effectively at an applied potential of −1.6 V _Ag/AgCl , yielding turnover numbers of 2,820 and 2,290, respectively, after 30 minutes. Species 3 lacked activity and was used as a negative control to eliminate the possibility of ligand‐based catalysis. Pre‐ and post‐catalytic data gave evidence of the molecular nature of the process within the timeframe of the experiments. Species 1 showed structural, rather than electronic cooperativity, while species 2 displayed no obvious cooperativity. DFT methods complemented the experimental results determining plausible mechanisms.

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Research Organization:: Wayne State Univ., Detroit, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE

Grant/Contract Number:: SC0001907; FG02-09ER16120; FOA0002414; CHE-1856437

OSTI ID:: 1976300

Alternate ID(s):: OSTI ID: 1859436

Journal Information:: Chemistry - A European Journal, Vol. 28, Issue 23; ISSN 0947-6539

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
water reduction
proton reduction
bimetallic cooperativity
cobalt catalysts
nickel catalysts
zinc complexes

CCDC 2112778: Experimental Crystal Structure Determination Fredricka, Morgan,; Richard, Schaugaard,; Dennis, Anderson, https://doi.org/10.5517/ccdc.csd.cc28xj4w The current record is supplemented by this dataset	dataset	January 2022
CCDC 2112779: Experimental Crystal Structure Determination Fredricka, Morgan,; Richard, Schaugaard,; Dennis, Anderson, https://doi.org/10.5517/ccdc.csd.cc28xj5x The current record is supplemented by this dataset	dataset	January 2022
CCDC 2112780: Experimental Crystal Structure Determination Fredricka, Morgan,; Richard, Schaugaard,; Dennis, Anderson, https://doi.org/10.5517/ccdc.csd.cc28xj6y The current record is supplemented by this dataset	dataset	January 2022

Title: Distinct Bimetallic Cooperativity Among Water Reduction Catalysts Containing [CoIIICoIII], [NiIINiII], and [ZnIIZnII] Cores

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