Co, Fe, and Mn in La-perovskite oxides for low temperature thermochemical CO2 conversion
Co, Fe, and Mn in La-perovskite oxides for low temperature thermochemical CO2 conversion
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DOI：
10.1016/j.cattod.2019.04.028
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发表时间：
2019-11-01
期刊：
影响因子：
5.3
通讯作者：
Bhethanabotla, Venkat R.
中科院分区：
文献类型：
--
作者：
Ramos, Adela E.;Maiti, Debtanu;Bhethanabotla, Venkat R.
ABO(3)形式的钙钛矿氧化物在低温热化学CO2转化为CO的逆水气移化学循环（RWGS-CL）工艺中显示出巨大的前景。这些钙钛矿氧化物“B”位上的过渡金属是调整材料性质的关键，这对有效的CO2转化至关重要。通过理论和实验相结合的方法研究了Co、Fe和Mn在LaBO3中的作用。通过从头算密度泛函理论（ab-initio density functional theory， DFT）模拟研究了这些材料的本征氧空位形成特征和电子电荷分布，并通过实验研究了这些材料的微尺度性质，如晶体尺寸和CO2转化率。通过这项多尺度研究，区分了富铁钙钛矿相对于富Co和富Mn相稳定和增强CO2转化现象的材料性质。
Perovskite oxides of the form ABO(3) have shown substantial promise in reverse water gas shift chemical looping (RWGS-CL) process for low temperature thermochemical CO2 conversion to CO. Transition metals on the 'B' site of these perovskite oxides hold the key to tuning the material properties essential for efficient CO2 conversion. The role of Co, Fe and Mn in LaBO3 has been investigated through a combined theoretical and experimental approach. Intrinsic oxygen vacancy formation characteristics of these materials and the electronic charge distribution were explored via ab-initio density functional theory (DFT) simulations, while the microscale properties like crystallite size and CO2 conversion yield were probed experimentally. Through this multiscale study, the material properties that govern the stable and enhanced CO2 conversion phenomenon by Fe rich perovskites as opposed to Co and Mn rich phases are differentiated.