Redox-Stable Electrodes for Ethane Dehydrogenation Based on Proton Ceramic Electrochemical Reactors

IF 5.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL
Elena Barrio-Querol, Laura Almar, David Catalán-Martínez, Kwati Leonard, José Manuel Serra* and Sonia Escolástico*, 
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Abstract

Ethylene is one of the most widely used components in the chemical industry, but the main manufacturing route involves significant energy consumption and generates substantial CO2 emissions. Proton ceramic electrochemical reactors (PCERs) offer great potential for process intensification and could play a key role in ethane dehydrogenation (EDH) by extracting H2 produced during the reaction. This process not only improves the reaction yield but also enables the production of a pure separated H2 stream. However, nonoxidative EDH reaction conditions lead to coke formation, which is further increased by H2 extraction, resulting in a decrease in system performance. Therefore, to successfully integrate PCER technology into ethylene production, it is crucial to develop stable redox electrodes that can withstand both nonoxidative H2 extraction and coke oxidation conditions. In this work, we study different composite electrodes based on the perovskite La0.8Sr0.2Cr0.5Mn0.5O3−δ (LSCM) combined with the proton conductor BaCe0.55Zr0.3Y0.15O3−δ (BCZY5515). The electrochemical performance was characterized by using electrochemical impedance spectroscopy under both oxidizing and reducing conditions. The data analysis indicates that surface processes limit electrode operation. The infiltration of Pt and CeO2 nanoparticles in the electrode enhanced the electrochemical performance, improving it by a factor of 10 at 700 °C. The optimal electrochemical performance was observed for the LSCMF/BCZY5515 (La0.8Sr0.2Cr0.5Mn0.25Fe0.25O3−δ/BaCe0.55Zr0.3Y0.15O3−δ) electrode infiltrated with Pt/CeO2, demonstrating promising properties as a redox-stable electrode. Finally, we evaluated the nonoxidative EDH reaction using a PCER based on a Ni–SrZr0.5Ce0.4Y0.1O2.95 (SZCY541) supported cell with a LSCMF/BCZY5515 anode infiltrated with Pt/CeO2 and a thin BaZr0.44Ce0.36Y0.2O3−δ electrolyte.

乙烯是化学工业中应用最广泛的成分之一,但其主要生产工艺需要消耗大量能源,并产生大量二氧化碳排放。质子陶瓷电化学反应器(PCER)为工艺强化提供了巨大潜力,通过提取反应过程中产生的 H2,可在乙烷脱氢(EDH)中发挥关键作用。这种工艺不仅能提高反应产率,还能产生纯净的分离 H2 流。然而,非氧化乙烷脱氢反应条件会导致焦炭的形成,而 H2 萃取又会进一步增加焦炭的形成,从而导致系统性能下降。因此,要成功地将 PCER 技术集成到乙烯生产中,关键是要开发出既能承受非氧化性 H2 萃取又能承受焦炭氧化条件的稳定氧化还原电极。在这项工作中,我们研究了基于包晶 La0.8Sr0.2Cr0.5Mn0.5O3-δ (LSCM) 与质子导体 BaCe0.55Zr0.3Y0.15O3-δ (BCZY5515) 的不同复合电极。在氧化和还原条件下,利用电化学阻抗谱对其电化学性能进行了表征。数据分析表明,表面过程限制了电极的运行。在电极中渗入铂和 CeO2 纳米粒子可提高电化学性能,在 700 °C 时可提高 10 倍。渗入了 Pt/CeO2 的 LSCMF/BCZY5515 (La0.8Sr0.2Cr0.5Mn0.25Fe0.25O3-δ/BaCe0.55Zr0.3Y0.15O3-δ)电极的电化学性能最佳,显示出作为氧化还原稳定电极的良好特性。最后,我们使用基于 Ni-SrZr0.5Ce0.4Y0.1O2.95 (SZCY541) 支撑电池的 PCER 评估了非氧化性 EDH 反应,该电池的阳极为 LSCMF/BCZY5515,渗入了 Pt/CeO2 和 BaZr0.44Ce0.36Y0.2O3-δ 薄电解质。
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来源期刊
ACS Applied Energy Materials
ACS Applied Energy Materials Materials Science-Materials Chemistry
CiteScore
10.30
自引率
6.20%
发文量
1368
期刊介绍: ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.
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