Perovskites with in situ exsolved metal nanoparticles have been extensively studied for CO electrolysis in solid oxide electrolysis cell. However, exsolution process is strongly governed by the sluggish diffusion rate of cations and poor structural stability issues. Here we present a new exsolution process on redox stable PrSrCrNiO (PSCN) perovskite by topotactic exsolution. This process tends to generate host stoichiometric PrSrCr(FeNi)O perovskite, triggering Ni cations segregation from the host while maintaining structural stability via supplement of Fe guest cations. The FeNi alloy nanoparticles decorated cathode showed a current density of 1.49 A cm at 800 °C and 1.6 V for CO electrolysis, demonstrating over 62.0 % improvement compared to the primitive PSCN cathode. Experimental studies and density functional theory calculations revealed that the activity originated from the unique ability to adsorb and activate CO at the metal/perovskite interfaces. This cation supplement strategy may expand the frontiers in the evolution of exsolution on perovskite catalysts for CO utilization and other heterogeneous catalytic reactions.

中文翻译：

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通过在 Pr0.7Sr0.3Cr0.9Ni0.1O3−δ 钙钛矿上的拓扑阳离子交换，铁触发 FeNi 合金纳米颗粒的溶出，用于 ​​CO2 电解


原位溶解金属纳米颗粒的钙钛矿已被广泛研究用于固体氧化物电解池中的 CO 电解。然而，出溶过程很大程度上受到阳离子扩散速率缓慢和结构稳定性差问题的影响。在这里，我们提出了一种通过拓扑脱溶对氧化还原稳定的 PrSrCrNiO (PSCN) 钙钛矿进行脱溶的新工艺。该过程往往会生成主体化学计量的 PrSrCr(FeNi)O 钙钛矿，引发 Ni 阳离子从主体中分离，同时通过补充 Fe 客体阳离子来保持结构稳定性。 FeNi合金纳米粒子装饰的阴极在800°C和1.6V的CO电解条件下表现出1.49A·cm的电流密度，与原始PSCN阴极相比提高了62.0％以上。实验研究和密度泛函理论计算表明，该活性源于金属/钙钛矿界面独特的吸附和活化CO的能力。这种阳离子补充策略可能会扩大用于CO利用和其他多相催化反应的钙钛矿催化剂的溶出演化的前沿。