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基于质子陶瓷电化学反应器的用于乙烷脱氢的氧化还原稳定电极

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

作者信息

Barrio-Querol Elena, Almar Laura, Catalán-Martínez David, Leonard Kwati, Serra José Manuel, Escolástico Sonia

机构信息

Instituto de Tecnología Química (Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas), València 46022, Spain.

Center for Energy Systems Design (CESD), International Institute for Carbon-Neutral Energy Research (I2CNER), Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan.

出版信息

ACS Appl Energy Mater. 2025 Mar 27;8(7):4345-4354. doi: 10.1021/acsaem.4c03281. eCollection 2025 Apr 14.

DOI:10.1021/acsaem.4c03281
PMID:40248401
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12001183/
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 CO emissions. Proton ceramic electrochemical reactors (PCERs) offer great potential for process intensification and could play a key role in ethane dehydrogenation (EDH) by extracting H produced during the reaction. This process not only improves the reaction yield but also enables the production of a pure separated H stream. However, nonoxidative EDH reaction conditions lead to coke formation, which is further increased by H 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 H extraction and coke oxidation conditions. In this work, we study different composite electrodes based on the perovskite LaSrCrMnO (LSCM) combined with the proton conductor BaCeZrYO (BCZY). 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 CeO 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/BCZY (LaSrCrMnFeO/BaCeZrYO) electrode infiltrated with Pt/CeO, demonstrating promising properties as a redox-stable electrode. Finally, we evaluated the nonoxidative EDH reaction using a PCER based on a Ni-SrZrCeYO (SZCY541) supported cell with a LSCMF/BCZY anode infiltrated with Pt/CeO and a thin BaZrCeYO electrolyte.

摘要

乙烯是化学工业中使用最广泛的成分之一，但主要制造路线涉及大量能源消耗并产生大量一氧化碳排放。质子陶瓷电化学反应器（PCER）在过程强化方面具有巨大潜力，并且通过提取反应过程中产生的氢气，在乙烷脱氢（EDH）中可以发挥关键作用。这个过程不仅提高了反应产率，还能生产出纯净的分离氢气流。然而，非氧化EDH反应条件会导致焦炭形成，而氢气提取会进一步加剧焦炭形成，从而导致系统性能下降。因此，要成功将PCER技术整合到乙烯生产中，开发能够承受非氧化氢气提取和焦炭氧化条件的稳定氧化还原电极至关重要。在这项工作中，我们研究了基于钙钛矿LaSrCrMnO（LSCM）与质子导体BaCeZrYO（BCZY）的不同复合电极。通过在氧化和还原条件下使用电化学阻抗谱对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。电极中铂和氧化铈纳米颗粒的渗透增强了电化学性能，在700℃时将其提高了10倍。对于渗透有Pt/CeO的LSCMF/BCZY（LaSrCrMnFeO/BaCeZrYO）电极，观察到了最佳的电化学性能，显示出作为氧化还原稳定电极的良好性能。最后，我们使用基于Ni-SrZrCeYO（SZCY541）支撑电池的PCER评估了非氧化EDH反应，该电池具有渗透有Pt/CeO的LSCMF/BCZY阳极和薄的BaZrCeYO电解质。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/906b1d692b89/ae4c03281_0009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/daa76d533b83/ae4c03281_0001.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/906b1d692b89/ae4c03281_0009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/daa76d533b83/ae4c03281_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/4b255fe5ecd2/ae4c03281_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/8f9d3fbb1a3f/ae4c03281_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/5b56403a0b73/ae4c03281_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/7e0aedccf93b/ae4c03281_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/a6f1d40c72db/ae4c03281_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/6c1d47529020/ae4c03281_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/327f2ca55950/ae4c03281_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/40ce/12001183/906b1d692b89/ae4c03281_0009.jpg

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本文引用的文献

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Single-step hydrogen production from NH, CH, and biogas in stacked proton ceramic reactors.在堆叠质子陶瓷反应器中，从 NH、CH 和沼气中一步制氢。
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