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Atomic-level Cu active sites enable energy-efficient CO2 electroreduction to multicarbon products in strong acid

  • Lizhou Fan,
  • Feng Li,
  • Tianqi Liu,
  • Jianan Erick Huang,
  • Rui Kai Miao,
  • Yu Yan,
  • Shihui Feng,
  • Cheuk-Wai Tai,
  • Sung-Fu Hung,
  • Hsin-Jung Tsai,
  • Meng-Cheng Chen,
  • Yang Bai,
  • Dongha Kim,
  • Sungjin Park,
  • Panos Papangelakis,
  • Chengqian Wu,
  • Ali Shayesteh Zeraati,
  • Roham Dorakhan,
  • Licheng Sun,
  • David Sinton,
  • Edward Sargent

摘要

Electrochemical CO2 reduction provides a promising strategy to synthesize C2+ compounds with reduced carbon intensity; however, high overall energy consumption restricts practical implementation. Using acidic media enables high CO2 utilization and low liquid product crossover, but to date has suffered low C2+ product selectivity. Here we hypothesize that adjacent pairs of atomic-copper active sites may favour C–C coupling, thus facilitating C2+ product formation. We construct tandem electrocatalysts with two distinct classes of active sites, the first for CO2 to CO, and the second, a dual-atomic-site catalyst, for CO to C2+. This leads to an ethanol Faradaic efficiency of 46% and a C2+ product Faradaic efficiency of 91% at 150 mA cm2 in an acidic CO2 reduction reaction. We document a CO2 single-pass utilization of 78% and an energy efficiency of 30% towards C2+ products; an ethanol crossover rate of 5%; and an ethanol product concentration of 4.5%, resulting in an exceptionally low projected energy cost of 249 GJ t−1 for the electrosynthesis of ethanol via the CO2 reduction reaction.