Direct propylene epoxidation via water activation over Pd-Pt electrocatalysts

• 成果类型: Article
• 署名作者: Chung, Minju; Maalouf, Joseph H.; Adams, Jason S.; Jiang, Chenyu; Roman-Leshkov, Yuriy; Manthiram, Karthish
• 署名单位: Massachusetts Institute of Technology (MIT); California Institute of Technology
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-8574
• DOI: 10.1126/science.adh4355
• 发表日期: 2024-01-05
• 页码: 49-55
• 关键词: oxygen; propene; nanoparticles; platinum(ii); alkenes; oxides

摘要

Direct electrochemical propylene epoxidation by means of water-oxidation intermediates presents a sustainable alternative to existing routes that involve hazardous chlorine or peroxide reagents. We report an oxidized palladium-platinum alloy catalyst (PdPtOx/C), which reaches a Faradaic efficiency of 66 +/- 5% toward propylene epoxidation at 50 milliamperes per square centimeter at ambient temperature and pressure. Embedding platinum into the palladium oxide crystal structure stabilized oxidized platinum species, resulting in improved catalyst performance. The reaction kinetics suggest that epoxidation on PdPtOx/C proceeds through electrophilic attack by metal-bound peroxo intermediates. This work demonstrates an effective strategy for selective electrochemical oxygen-atom transfer from water, without mediators, for diverse oxygenation reactions.