Revealing the Influence of Diverse Secondary Metal Cations on Redox-Active Palladium Complexes

Golwankar, Riddhi R.; Kumar, Amit; Day, Victor W.; Blakemore, James D.

doi:10.1002/chem.202200344

Title: Revealing the Influence of Diverse Secondary Metal Cations on Redox-Active Palladium Complexes

Journal Article · 07 April 2022 · Chemistry - A European Journal

DOI: https://doi.org/10.1002/chem.202200344 · OSTI ID:1976301

^[1];

^[1]; Day, Victor W. ^[1];

^[1]

University of Kansas, Lawrence, KS (United States)

Abstract Incorporation of redox‐inactive metals into redox‐active complexes and catalysts attracts attention for engendering new reactivity modes, but this strategy has not been extensively investigated beyond the first‐row of the transition metals. Here, the isolation and characterization of the first series of heterobimetallic complexes of palladium with mono‐, di‐, and tri‐valent redox‐inactive metal ions are reported. A Reinhoudt‐type heteroditopic ligand with a salen‐derived [ N ₂ , O ₂ ] binding site for Pd and a crown‐ether‐derived [ O ₆ ] site has been used to prepare isolable adducts of the Lewis acidic redox‐inactive metal ions ( M ⁿ⁺ ). Comprehensive data from single‐crystal X‐ray diffraction analysis reveal distinctive trends in the structural properties of the heterobimetallic species, including an uncommon dependence of the Pd⋅⋅⋅ M distance on Lewis acidity. The reorganization energy associated with reduction of the heterobimetallic species is strongly modulated by Lewis acidity, with the slowest heterogeneous electron transfer kinetics associated with the strongest incorporated Lewis acids. This hitherto unexplored reorganization energy penalty for electron transfer contrasts with prior thermodynamic studies, revealing that kinetic parameters should be considered in studies of reactivity involving heterobimetallic species.

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Research Organization:: Univ. of Kansas, Lawrence, KS (United States)

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

Grant/Contract Number:: SC0019169

OSTI ID:: 1976301

Alternate ID(s):: OSTI ID: 1869743

Journal Information:: Chemistry - A European Journal, Vol. 28, Issue 38; ISSN 0947-6539

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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CCDC 2056710: Experimental Crystal Structure Determination R., Golwankar, Riddhi; Amit, Kumar,; W., Day, Victor https://doi.org/10.5517/ccdc.csd.cc2715hz The current record is supplemented by this dataset	dataset	January 2022
CCDC 2056711: Experimental Crystal Structure Determination R., Golwankar, Riddhi; Amit, Kumar,; W., Day, Victor https://doi.org/10.5517/ccdc.csd.cc2715j0 The current record is supplemented by this dataset	dataset	January 2022
CCDC 2056712: Experimental Crystal Structure Determination R., Golwankar, Riddhi; Amit, Kumar,; W., Day, Victor https://doi.org/10.5517/ccdc.csd.cc2715k1 The current record is supplemented by this dataset	dataset	January 2022
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CCDC 2056714: Experimental Crystal Structure Determination R., Golwankar, Riddhi; Amit, Kumar,; W., Day, Victor https://doi.org/10.5517/ccdc.csd.cc2715m3 The current record is supplemented by this dataset	dataset	January 2022
CCDC 2056715: Experimental Crystal Structure Determination R., Golwankar, Riddhi; Amit, Kumar,; W., Day, Victor https://doi.org/10.5517/ccdc.csd.cc2715n4 The current record is supplemented by this dataset	dataset	January 2022
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CCDC 2056718: Experimental Crystal Structure Determination R., Golwankar, Riddhi; Amit, Kumar,; W., Day, Victor https://doi.org/10.5517/ccdc.csd.cc2715r7 The current record is supplemented by this dataset	dataset	January 2022