<p>Direct electrochemical ethylene (C<sub>2</sub>H<sub>4</sub>) epoxidation with water (H<sub>2</sub>O) represents a promising approach for the production of value-added ethylene oxide (EO) in a sustainable way. However, the activity remains limited due to the sluggish activation of C<sub>2</sub>H<sub>4</sub> and the stiff formation of *OH intermediate. This paper describes the design of a Ag/SnO<sub>2</sub> electrocatalyst to achieve efficient electrochemical C<sub>2</sub>H<sub>4</sub> epoxidation with a high faradaic efficiency of 39.4% for EO and a high selectivity of 91.5% at 25 mA/cm<sup>2</sup> in a membrane electrode assembly. Results of in&#xa0;situ attenuated total reflection infrared spectra characterizations and computational calculations reveal that the Ag/SnO<sub>2</sub> interface promotes C<sub>2</sub>H<sub>4</sub> adsorption and activation to obtain *C<sub>2</sub>H<sub>4</sub>. Moreover, electrophilic *OH is generated on the catalyst surface through H<sub>2</sub>O dissociation, which further reacts with *C<sub>2</sub>H<sub>4</sub> to facilitate the formation of *C<sub>2</sub>H<sub>4</sub>OH, contributing to the enhanced electrochemical epoxidation activity. This work would provide general guidance for designing catalysts for electrochemical olefin epoxidation through interface engineering.</p>

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Electrochemical epoxidation enhanced by C2H4 activation and hydroxyl generation at the Ag/SnO2 interface

  • Hao Dong,
  • Ran Luo,
  • Gong Zhang,
  • Lulu Li,
  • Chaoxi Wang,
  • Guodong Sun,
  • Hongyi Wang,
  • Jiachang Liu,
  • Tuo Wang,
  • Zhi-Jian Zhao,
  • Peng Zhang,
  • Jinlong Gong

摘要

Direct electrochemical ethylene (C2H4) epoxidation with water (H2O) represents a promising approach for the production of value-added ethylene oxide (EO) in a sustainable way. However, the activity remains limited due to the sluggish activation of C2H4 and the stiff formation of *OH intermediate. This paper describes the design of a Ag/SnO2 electrocatalyst to achieve efficient electrochemical C2H4 epoxidation with a high faradaic efficiency of 39.4% for EO and a high selectivity of 91.5% at 25 mA/cm2 in a membrane electrode assembly. Results of in situ attenuated total reflection infrared spectra characterizations and computational calculations reveal that the Ag/SnO2 interface promotes C2H4 adsorption and activation to obtain *C2H4. Moreover, electrophilic *OH is generated on the catalyst surface through H2O dissociation, which further reacts with *C2H4 to facilitate the formation of *C2H4OH, contributing to the enhanced electrochemical epoxidation activity. This work would provide general guidance for designing catalysts for electrochemical olefin epoxidation through interface engineering.