Electrochemical promotion of catalysis controlled by chemical potential difference across a mixed ionic-electronic conducting ceramic membrane - an example of wireless NEMCA

被引:24
作者
Poulidi, D. [1 ]
Thursfield, A. [1 ]
Metcalfe, I. S. [1 ]
机构
[1] Newcastle Univ, Dept Chem Engn & Adv Mat, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England
关键词
electrochemical promotion; chemical potential difference; surface oxygen capture; MIEC membrane; La0.6Sr0.4Co0.2F0.8O3; ethylene oxidation;
D O I
10.1007/s11244-006-0136-0
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
A La0.6Sr0.4Co0.2F0.8O3 mixed ionic electronic conducting (MIEC) membrane was used in a dual chamber reactor for the promotion of the catalytic activity of a platinum catalyst for ethylene oxidation. By controlling the oxygen chemical potential difference across the membrane, a driving force for oxygen ions to migrate across the membrane and backspillover onto the catalyst surface is established. The reaction is then promoted by the formation of a double layer of oxide anions on the catalyst surface. The electronic conductivity of the membrane material eliminates the need for an external circuit to pump the promoting oxide ion species through the membrane and onto the catalyst surface. This renders this "wireless" system simpler and more amenable for large-scale practical application. Preliminary experiments show that the reaction rate of ethylene oxidation can indeed be promoted by almost one order of magnitude upon exposure to an oxygen atmosphere on the sweep side of the membrane reactor, and thus inducing an oxygen chemical potential difference across the membrane, as compared to the rate under an inert sweep gas. Moreover, the rate does not return to its initial unpromoted value upon cessation of the oxygen flow on the sweep side, but remains permanently promoted. A number of comparisons are drawn between the classical electrochemical promotion that utilises an external circuit and the "wireless" system that utilises chemical potential differences. In addition a 'surface oxygen capture' model is proposed to explain the permanent promotion of the catalyst activity.
引用
收藏
页码:435 / 449
页数:15
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