Incorporation of a Metal Catalyst for the Ammonia Synthesis in a Ferroelectric Packed-Bed Plasma Reactor: Does It Really Matter?

材料科学 催化作用 氨生产 填充床 颗粒 铁电性 化学工程 锆钛酸铅 涂层 介质阻挡放电 图层(电子) 产量(工程) 无机化学 电介质 纳米技术 复合材料 化学 有机化学 光电子学 工程类
作者
Paula Navascués,Juan Garrido-García,José Cotrino,Agustín R. González‐Elipe,Ana Gómez‐Ramírez
出处
期刊:ACS Sustainable Chemistry & Engineering [American Chemical Society]
卷期号:11 (9): 3621-3632 被引量:16
标识
DOI:10.1021/acssuschemeng.2c05877
摘要

Plasma-catalysis has been proposed as a potential alternative for the synthesis of ammonia. Studies in this area focus on the reaction mechanisms and the apparent synergy existing between processes occurring in the plasma phase and on the surface of the catalytic material. In the present study, we approach this problem using a parallel-plate packed-bed reactor with the gap between the electrodes filled with pellets of lead zirconate titanate (PZT), with this ferroelectric material modified with a coating layer of alumina (i.e., Al2O3/PZT) and the same alumina layer incorporating ruthenium nanoparticles (i.e., Ru-Al2O3/PZT). At ambient temperature, the electrical behavior of the ferroelectric packed-bed reactor differed for these three types of barriers, with the plasma current reaching a maximum when using Ru-Al2O3/PZT pellets. A systematic analysis of the reaction yield and energy efficiency for the ammonia synthesis reaction, at ambient temperature and at 190 °C and various electrical operating conditions, has demonstrated that the yield and the energy efficiency for the ammonia synthesis do not significantly improve when including ruthenium particles, even at temperatures at which an incipient catalytic activity could be inferred. Besides disregarding a net plasma-catalysis effect, reaction results highlight the positive role of the ferroelectric PZT as moderator of the discharge, that of Ru particles as plasma hot points, and that of the Al2O3 coating as a plasma cooling dielectric layer.

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