Electrocatalytic hydrogenation of acetonitrile to ethylamine in acid.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 38622140.
- Also identified by DOI 10.1038/s41467-024-47622-9 and PMC identifier 11018601.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Electrochemical hydrogenation of acetonitrile based on well-developed proton exchange membrane electrolyzers holds great promise for practical production of ethylamine. However, the local acidic condition of proton exchange membrane results in severe competitive proton reduction reaction and poor selection toward acetonitrile hydrogenation. Herein, we conduct a systematic study to screen various metallic catalysts and discover Pd/C exhibits a 43.8% ethylamine Faradaic efficiency at the current density of 200 mA cm<sup>-2</sup> with a specific production rate of 2912.5 mmol g<sup>-1</sup> h<sup>-1</sup>, which is about an order of magnitude higher than the other screened metal catalysts. Operando characterizations indicate the in-situ formed PdH<sub>x</sub> is the active centers for catalytic reaction and the adsorption strength of the *MeCH<sub>2</sub>NH<sub>2</sub> intermediate dictates the catalytic selectivity. More importantly, the theoretical analysis reveals a classic d-band mediated volcano curve to describe the relation between the electronic structures of catalysts and activity, which could provide valuable insights for designing more effective catalysts for electrochemical hydrogenation reactions and beyond.