Literature DB >> 29676578

Countercations and Solvent Influence CO2 Reduction to Oxalate by Chalcogen-Bridged Tricopper Cyclophanates.

Brian J Cook, Gianna N Di Francesco, Khalil A Abboud, Leslie J Murray.   

Abstract

One-electron reduction of Cu3EL (L3- = tris(β-diketiminate)cyclophane, and E = S, Se) affords [Cu3EL]-, which reacts with CO2 to yield exclusively C2O42- (95% yield, TON = 24) and regenerate Cu3EL. Stopped-flow UV/visible data support an A→B mechanism under pseudo-first-order conditions ( kobs, 298K = 115(2) s-1), which is 106 larger than those for reported copper complexes. The kobs values are dependent on the countercation and solvent (e.g., kobs is greater for [K(18-crown-6)]+ vs (Ph3P)2N+, and there is a 20-fold decrease in kobs in THF vs DMF). Our results suggest a mechanism in which cations and solvent influence the stability of the transition state.

Entities:  

Year:  2018        PMID： 29676578     DOI： 10.1021/jacs.8b02508

Source DB:  PubMed          Journal:  J Am Chem Soc        ISSN： 0002-7863            Impact factor:   15.419


  7 in total

1.  Isolation of chloride- and hydride-bridged tri-iron and -zinc clusters in a tris(β-oxo-δ-diimine) cyclophane ligand.

Authors:  Dae Ho Hong; Brian J Knight; Vincent J Catalano; Leslie J Murray
Journal:  Dalton Trans       Date:  2019-07-02       Impact factor: 4.390

2.  Cyclophanes as Platforms for Reactive Multimetallic Complexes.

Authors:  Ricardo B Ferreira; Leslie J Murray
Journal:  Acc Chem Res       Date:  2019-01-22       Impact factor: 22.384

3.  Synthetic Factors Governing Access to Tris(β-diketimine) Cyclophanes versus Tripodal Tri-β-aminoenones.

Authors:  Mary C Eaton; Brian J Knight; Robin Brahmi; Ricardo B Ferreira; Vincent J Catalano; Arnold L Rheingold; Ion Ghiviriga; Leslie J Murray
Journal:  J Org Chem       Date:  2020-10-27       Impact factor: 4.354

Review 4.  Mechanisms of catalytic reduction of CO2 with heme and nonheme metal complexes.

Authors:  Shunichi Fukuzumi; Yong-Min Lee; Hyun S Ahn; Wonwoo Nam
Journal:  Chem Sci       Date:  2018-07-02       Impact factor: 9.825

5.  Oxalate production via oxidation of ascorbate rather than reduction of carbon dioxide.

Authors:  Fatemeh Khamespanah; Maximilian Marx; David B Crochet; Uttam R Pokharel; Frank R Fronczek; Andrew W Maverick; Matthias Beller
Journal:  Nat Commun       Date:  2021-03-25       Impact factor: 14.919

6.  Revisiting Reduction of CO2 to Oxalate with First-Row Transition Metals: Irreproducibility, Ambiguous Analysis, and Conflicting Reactivity.

Authors:  Maximilian Marx; Holm Frauendorf; Anke Spannenberg; Helfried Neumann; Matthias Beller
Journal:  JACS Au       Date:  2022-02-14

Review 7.  Molecular Catalysts for the Reductive Homocoupling of CO2 towards C2+ Compounds.

Authors:  Hong-Qing Liang; Torsten Beweries; Robert Francke; Matthias Beller
Journal:  Angew Chem Int Ed Engl       Date:  2022-03-24       Impact factor: 16.823
  7 in total

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