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Selective catalytic two-step process for ethylene glycol from carbon monoxide.

Kaiwu DongSaravanakumar ElangovanRui SangAnke SpannenbergRalf JackstellKathrin JungeYuehui LiMatthias Beller
Published in: Nature communications (2016)
Upgrading C1 chemicals (for example, CO, CO/H2, MeOH and CO2) with C-C bond formation is essential for the synthesis of bulk chemicals. In general, these industrially important processes (for example, Fischer Tropsch) proceed at drastic reaction conditions (>250 °C; high pressure) and suffer from low selectivity, which makes high capital investment necessary and requires additional purifications. Here, a different strategy for the preparation of ethylene glycol (EG) via initial oxidative coupling and subsequent reduction is presented. Separating coupling and reduction steps allows for a completely selective formation of EG (99%) from CO. This two-step catalytic procedure makes use of a Pd-catalysed oxycarbonylation of amines to oxamides at room temperature (RT) and subsequent Ru- or Fe-catalysed hydrogenation to EG. Notably, in the first step the required amines can be efficiently reused. The presented stepwise oxamide-mediated coupling provides the basis for a new strategy for selective upgrading of C1 chemicals.
Keyphrases
  • room temperature
  • ionic liquid
  • minimally invasive
  • electron transfer
  • mass spectrometry
  • crystal structure
  • molecularly imprinted
  • simultaneous determination
  • tandem mass spectrometry