A Tandem Electrocatalysis and Hydroformylation Approach to Synthesize High-Carbon Aldehydes from CO2

Abstract

The electrochemical CO2 reduction reaction (eCO2RR) typically yields low-carbon products (Cn, n≤3), thereby limiting its application scope. Herein, we design a cascaded eCO2RR-hydroformylation system for synthesizing high-carbon (C9) aldehydes from CO2. NixCo1-x@NCNT catalysts enable the production of syngas with a tunable H2/CO ratio ranging from 0 to 5.3 using CO2 and H2O as feedstocks. Subsequently, Rh-based complexes are constructed to catalyze the downstream phenylacetylene hydroformylation. As a result, this tandem electrocatalysis-hydroformylation approach achieves a high phenylacetylene conversion efficiency of 87%, with aldehyde selectivity up to 53% under room pressure and temperature.