新型固体氧化物电解池阳极用于高效电催化甲烷氧化偶联OA
Novel solid oxide electrolysis cell anode for efficient electrocatalytic oxidative coupling of methane
开发了一类新型微通道结构 La0.6Sr0.4Co0.8Fe0.2O3+δ-(Ce0.9Gd0.1)O1.95(GDC)复合阳极,即微通道电极(MCE),并制备了 MCE 全电池,用于固体氧化物电解池(SOEC)中 CH4 电催化氧化偶联,利用 SEM、FTIR 和电化学性能测试等方法对MCE 的结构及 SOEC 的 CH4 转化性能进行了表征.实验结果表明,性能最优的 SOEC 在 850℃、2.0 V、200 mA/cm2 下电解纯 CH4 时,碳二产物选择性可达 70.6%,在 6 000 s 的运行过程中未见性能衰减.MCE 独特的微通道结构能提升 CH4 转化速率;而精准控制的电化学窗口可抑制 COx 副产物生成,提升碳二产物选择性.密度泛函理论计算证实,GDC 可提升活性氧物种 O22-的稳定性,促进 CH4 中 C—H 键断裂,同时抑制氧析出反应,稳定晶格结构.复合阳极的开发为 SOEC 新结构、高性能阳极的制备提供了新思路,对于CH4 的电化学转化和化工利用具有理论意义与应用价值.
The work developed a La0.6Sr0.4Co0.8Fe0.2O3+δ-(Ce0.9Gd0.1)O1.95(GDC)composite anode with a novel micro-channel structure(denoted as micro-channel electrode(MCE))and fabricated a solid oxide electrolysis cell(SOEC)based on the MCE to achieve electrocatalytic oxidative coupling of CH4.The structure of MCE and the CH4 conversion performance of SOEC were characterized by using SEM,FTIR,and electrochemical measurements.The results show that when electrolyzing pure CH4 at 850℃,2.0 V,and 200 mA/cm2,the optimal SOEC achieves a high C2 product selectivity of 70.6%with no significant performance degradation over 6 000 s.In situ high-temperature infrared spectroscopy confirms that the unique micro-channel structure of MCE enhances the CH4 conversion rate,while the precisely controlled potential window suppresses the production of COx,thereby improving C2 product selectivity.DFT calculations reveal that the GDC component stabilizes active oxygen species O22-,facilitates C—H bond cleavage in CH4,concurrently inhibits oxygen evolution reaction,and stabilizes the lattice structure.The development of this composite anode provides new insights for designing high-performance SOEC anodes with novel structures and advancing the electrochemical conversion and utilization of CH4.
欧阳瑞泽;白帆;张穆薇;李一枫
浙江大学 工程师学院,浙江 杭州 310015||中石化(北京)化工研究院有限公司,北京 100013中石化(北京)化工研究院有限公司,北京 100013中石化(北京)化工研究院有限公司,北京 100013中石化(北京)化工研究院有限公司,北京 100013
化学化工
固体氧化物电解池甲烷氧化偶联电催化原位红外光谱
solid oxide electrolysis celloxidative coupling of methaneelectrocatalysisin situ infrared spectroscopy
《石油化工》 2026 (6)
811-819,9
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