Revisiting Reduction of CO2to Oxalate with First-Row Transition Metals: Irreproducibility, Ambiguous Analysis, and Conflicting Reactivity

Maximilian Marx, Holm Frauendorf, Anke Spannenberg, Helfried Neumann, Matthias Beller

Research output: Contribution to journalArticlepeer-review

9 Scopus citations

Abstract

Construction of higher C≥2compounds from CO2constitutes an attractive transformation inspired by nature's strategy to build carbohydrates. However, controlled C-C bond formation from carbon dioxide using environmentally benign reductants remains a major challenge. In this respect, reductive dimerization of CO2to oxalate represents an important model reaction enabling investigations on the mechanism of this simplest CO2coupling reaction. Herein, we present common pitfalls encountered in CO2reduction, especially its reductive coupling, based on established protocols for the conversion of CO2into oxalate. Moreover, we provide an example to systematically assess these reactions. Based on our work, we highlight the importance of utilizing suitable orthogonal analytical methods and raise awareness of oxidative reactions that can likewise result in the formation of oxalate without incorporation of CO2. These results allow for the determination of key parameters, which can be used for tailoring of prospective catalytic systems and will promote the advancement of the entire field.

Original languageEnglish
Pages (from-to)731-744
Number of pages14
JournalJACS Au
Volume2
Issue number3
DOIs
StatePublished - 28 Mar 2022
Externally publishedYes

Keywords

  • COreduction
  • COreductive coupling
  • Cu catalysis
  • Fe catalysis
  • oxalic acid
  • oxidation

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