Symmetrical Exsolution of Rh Nanoparticles in Solid Oxide Cells for Efficient Syngas Production from Greenhouse Gases
Symmetrical Exsolution of Rh Nanoparticles in Solid Oxide Cells for Efficient Syngas Production from Greenhouse Gases
复制标题
DOI：
10.1021/acscatal.9b04424
复制
发表时间：
2020-01-17
期刊：
影响因子：
12.9
通讯作者：
Tsampas, Mihalis N.
中科院分区：
文献类型：
--
作者：
Kyriakou, Vasileios;Neagu, Dragos;Tsampas, Mihalis N.
二氧化碳和蒸汽固体氧化物共电解是利用可再生电力生产费托合成合成气原料的关键技术。该工艺与甲烷部分氧化在单个电池中的集成可以消除甚至逆转共电解的电力需求，同时以工业上有吸引力的 H-2/CO 比率生产合成气。然而，该系统相当复杂，需要具有催化活性和耐焦炭的电极。在这里，我们报告了用于该过程的低取代钛酸铑钙钛矿 (La0.43Ca0.32Rh0.06Ti094O3) 电极，能够溶解高 Rh 纳米颗粒群，并组装成对称的固体氧化物电池结构。通过将干燥甲烷引入阳极室，电力需求显着降低，甚至允许合成气和电力联产。为了进一步了解 Rh 纳米颗粒对甲烷转化为合成气的作用，我们通过改变钙钛矿的还原温度来调整它们的尺寸和数量。我们的结果例证了如何利用外解概念来有效地利用贵金属来在具有挑战性的能源相关应用中激活低反应性温室气体。
Carbon dioxide and steam solid oxide co-electrolysis is a key technology for exploiting renewable electricity to generate syngas feedstock for the Fischer-Tropsch synthesis. The integration of this process with methane partial oxidation in a single cell can eliminate or even reverse the electrical power demands of co-electrolysis, while simultaneously producing syngas at industrially attractive H-2/CO ratios. Nevertheless, this system is rather complex and requires catalytically active and coke tolerant electrodes. Here, we report on a low-substitution rhodium-titanate perovskite (La0.43Ca0.32Rh0.06Ti094O3) electrode for the process, capable of exsolving high Rh nanoparticle populations, and assembled in a symmetrical solid oxide cell configuration. By introducing dry methane to the anode compartment, the electricity demands are impressively decreased, even allowing syngas and electricity cogeneration. To provide further insight on the Rh nanoparticles role on methane-to-syngas conversion, we adjusted their size and population by altering the reduction temperature of the perovskite. Our results exemplify how the exsolution concept can be employed to efficiently exploit noble metals for activating low-reactivity greenhouse gases in challenging energy-related applications.