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- ItemSelective catalytic two-step process for ethylene glycol from carbon monoxide([London] : Nature Publishing Group UK, 2016) Dong, Kaiwu; Elangovan, Saravanakumar; Sang, Rui; Spannenberg, Anke; Jackstell, Ralf; Junge, Kathrin; Li, Yuehui; Beller, MatthiasUpgrading 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.
- ItemEarth-abundant photocatalytic systems for the visible-light-driven reduction of CO2 to CO(Cambridge : RSC, 2017) Rosas-Hernández, Alonso; Steinlechner, Christoph; Junge, Henrik; Beller, MatthiasHerein, we report a highly selective photocatalytic system, based on an in situ copper photosensitizer and an iron catalyst, for the reduction of CO2 to CO. Turnover numbers (TON) up to 487 (5 h) with selectivities up to 99% and ΦCO = 13.3% were observed. Stern-Volmer analysis allowed us to establish a reductive quenching mechanism between the Cu PS and electron donor.