化学
环氧乙烷
电解
乙烯
无机化学
催化作用
氧化物
电合成
电催化剂
电解质
环氧化物
乙二醇
多相催化
析氧
法拉第效率
化学工程
阳极
格式化
氧气
电化学
分离器(采油)
化学需氧量
甲醇
酒精氧化
作者
Jianan Erick Huang,Chengqian Wu,Yiqing Chen,Jiaqi Yu,Yuanjun Chen,Huajie Ze,Jaerim Kim,J K Y Wu,Yang Bai,Xiangyu Ma,Roham Dorakhan,Bosi Peng,Hongmin An,Rui Kai Miao,Min Liu,Lizhou Fan,Sungjin Park,Ke Xie,David Sinton,Edward H. Sargent
摘要
Demand for ethylene oxide (EO)─a chemical building block for plastics─exceeds 30 Mt/year. Electrosynthesis of EO from ethylene has, in the highest-activity reports to date, relied on redox-mediated approaches; these lead to chlorinated organic byproducts and high product separation costs due to dilution in solvents as a result of homogeneous electrochemistry. Direct electro-epoxidation is outcompeted by the oxygen evolution reaction (OER) at higher overpotential, causing faradaic efficiencies for EO to drop below 50% above 10 mA/cm 2 . We noted that the OER and ethylene oxidation share a common dependency on surface-adsorbed oxygen (M-O*), and that in Pt group metals, the stronger M-O* bonds enhance the kinetics of the OER relative to epoxidation. We therefore considered catalysts, such as Ag, having a less-strongly bound M-O* intermediate. Unfortunately, we found that Ag dissolved easily under anodic bias and that the oxidized Ag surface at a high oxidation state favors the overoxidation to CO 2 . We then aimed to leverage metal–support interactions, with our goal being to render the Ag more stable while in its higher oxidation state. An Ag-ZrO 2 catalyst synthesized from a MOF template coupled with the MEA-PTFE system achieves 50% FE for ethylene oxide at 50 mA/cm 2, with a productivity of 460 μmol cm –2 h –1 . The use of a hydrophilic PTFE separator minimizes system resistance, EO crossover, and hydrolysis, enabling an EO concentration of 48 wt % in the outlet stream at a full cell voltage of 2.1 V in electrolysis paired with HER.
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