Ye Lingting, Shang Zhibo, Xie Kui
Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
Key Laboratory of Design & Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
Angew Chem Int Ed Engl. 2022 Aug 8;61(32):e202207211. doi: 10.1002/anie.202207211. Epub 2022 Jun 24.
Catalytic conversion of CH to C H plays an important role in the light olefin industry. Here, we report the electrochemical conversion of CH to C H /C H at the anode with the electrolysis of CO to CO at the cathode in a solid oxide electrolyser. We constructed well-defined interfaces that function as three-phase boundaries by exsolving single-crystalline Ni nanoparticles in porous single-crystalline CeO monoliths. We engineered the chemical states and flux of active oxygen species for the oxidation of CH at the anode by controlling voltage and temperature. We show the unprecedented C selectivity (C H and C H ) of ≥99.5 % at a CH conversion of ≈7 %. The electrolyser exhibits excellent durability without performance degradation being observed in a continuous operation of 100 hours. Our work enables a novel path for the selective conversion of CH /CO into useful chemicals, and the technique of building well-defined interfaces may find potential applications in other fields.
将CH催化转化为C₂H₄在轻烯烃工业中起着重要作用。在此，我们报道了在固体氧化物电解槽中，通过在阴极将CO电解为CO₂，在阳极将CH电化学转化为C₂H₄/C₂H₆。我们通过在多孔单晶CeO整体材料中析出单晶Ni纳米颗粒，构建了作为三相边界起作用的明确界面。我们通过控制电压和温度来设计阳极上用于CH氧化的活性氧物种的化学状态和通量。我们展示了在CH转化率约为7%时，前所未有的≥99.5%的C₂H₄/C₂H₆选择性。该电解槽表现出优异的耐久性，在100小时的连续运行中未观察到性能下降。我们的工作为将CH₄/CO选择性转化为有用化学品开辟了一条新途径，构建明确界面的技术可能在其他领域找到潜在应用。
