V 2 O 5 Surface Electronic Structure Suppresses Ethane Over‐Oxidation, Enabling 65% Ethylene Yield

作者：Hongjuan Tao, Yan Chen, Suting He, Benchi Chen, Zhibo Shang, Zilin Ma, Xueming Liu, Liyuan Chai, Li Zhang · 发表于：Angewandte Chemie International Edition · 年份：2026 · DOI：10.1002/anie.8633105 · 被引用次数：1 · 研究领域：Catalysis and Oxidation Reactions、Electrocatalysts for Energy Conversion、Chemical Looping and Thermochemical Processes

ABSTRACT Electrochemical oxidative dehydrogenation (ODH) of ethane in solid oxide electrolysis cells (SOECs) offers an energy‐efficient route to ethylene but faces a trade‐off between conversion and selectivity due to over‐oxidation. Conventional voltage–current regulation can suppress deep oxidation but inevitably compromises ethane conversion. Here, we engineer surface electronic structures by depositing a V 2 O 5 layer on SrFe 0.9 Ti 0.1 O 3−δ (STF), introducing intrinsic O 2p (‐1.33 eV) and V 3d (‐0.18 eV) states closer to the Fermi level than in STF (‐1.49/‐4.52 eV). Density functional theory and operando infrared spectroscopy reveal three synergistic effects: enhanced ethane adsorption (Δ E ads ‐0.33 vs. ‐0.11 eV), reduced first dehydrogenation barrier (Δ G 1 1.13 vs. 1.15 eV), and promoted ethylene desorption ((Δ G des ‐Δ G 3 ) ‐4.98 vs. ‐1.92 eV). The optimized anode delivers 65% yield and 90% selectivity at 750°C, exceeding unmodified STF by 10%. This work highlights band‐center engineering as a promising design concept for regulating hydrocarbon electrode reactions.