In-situ Exsolution of Bimetallic CoFe nanoparticles on (La,Sr)FeO3 perovskite: Its effect on Electrocatalytic Oxidative Coupling of Methane
In-situ Exsolution of Bimetallic CoFe nanoparticles on (La,Sr)FeO3 perovskite: Its effect on Electrocatalytic Oxidative Coupling of Methane
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DOI：
10.1016/j.apcatb.2022.122026
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发表时间：
2022-10
期刊：
影响因子：
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通讯作者：
Jaesung Kim;Y. Kim;M. Ferree;S. Gunduz;A. Co;Minkyu Kim;U. Ozkan
中科院分区：
文献类型：
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作者：
Jaesung Kim;Y. Kim;M. Ferree;S. Gunduz;A. Co;Minkyu Kim;U. Ozkan
本研究提出了就地还原La-锶-钴铁氧体(LSCF)钙钛矿以改善其表面性质和提高其对甲烷氧化偶联(OCM)的电催化反应的有效方法。LSCF还原过程中杂相的演化导致了CoFe纳米颗粒在表面的形成。用于OCM的现场简化的LSCF电池可以在离子泵或燃料电池模式下运行。C2+烃和C3H6的高选择性分别为63%和10.2%。对LSCF和COFE的密度泛函计算表明，C2+烃在LSCF上的高选择性主要源于CoFe纳米粒子的存在；在CH4下进行的DRIFTS实验证明，通过降低LSCF可以有效地抑制CH4的完全氧化，控制供氧量是CH4选择性转化为高阶烃的重要参数。
This study presentsin-situreduction of lanthanum strontium cobalt ferrite (LSCF) perovskite as an effective method for modifying its surface properties and enhancing its electrocatalytic reactivity for oxidative coupling of methane (OCM). The evolution of hetero-phases during the reduction of LSCF resulted in CoFe nanoparticles being formed at the surface. Thein-situreduced LSCF cell for OCM could be operated in either an ion pump or a fuel cell mode. High selectivity of 63% and 10.2% were reported for C2+hydrocarbons and C3H6, respectively. DFT calculations on LSCF and CoFe revealed that the high selectivity of C2+hydrocarbons on the LSCF primarily stems from the presence of CoFe nanoparticles.In-situDRIFTS conducted under CH4proved that complete oxidation of CH4can be effectively inhibited by reducing LSCF, and control of oxygen supply is an important parameter for selective conversion of CH4to higher order hydrocarbon.