Lanthanum–Strontium–Manganese Perovskites as Redox Materials for Solar Thermochemical Splitting of H2O and CO2
Lanthanum–Strontium–Manganese Perovskites as Redox Materials for Solar Thermochemical Splitting of H2O and CO2
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DOI：
10.1021/ef301923h
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发表时间：
2013-03
期刊：
影响因子：
5.3
通讯作者：
J. Scheffe;David Weibel;A. Steinfeld
中科院分区：
文献类型：
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作者：
J. Scheffe;David Weibel;A. Steinfeld
对一类新的太阳热化学氧化还原中间体，即镧锶锰钙钛矿进行了热力学和实验研究。基于低温氧非化学计量数据的缺陷模型的制定和外推到更高的温度更相关的热化学氧化还原循环。在1523-1923 K温度范围内，La 1-xSrxMnO 3 −δ中Sr含量为x = 0.3（LSM 30）和x = 0.4（LSM 40）时的还原程度优于CeO 2。用CO2和H2O氧化在化学上不是有利的，并且在很大程度上取决于氧化剂浓度。该模型通过在高温（>1623 K）下的O2非化学计量测量和使用市售LSM 35的CO2还原循环进行实验验证。LSM 40和氧化铈氧化还原循环的理论太阳能-燃料能量转换效率在1800 K时分别为16和22%，在1600 K时分别为13和7%。
A thermodynamic and experimental investigation of a new class of solar thermochemical redox intermediates, namely, lanthanum–strontium–manganese perovskites, is presented. A defect model based on low-temperature oxygen non-stoichiometry data is formulated and extrapolated to higher temperatures more relevant to thermochemical redox cycles. Strontium contents of x = 0.3 (LSM30) and x = 0.4 (LSM40) in La1–xSrxMnO3−δ result in favorable reduction extents compared to ceria in the temperature range of 1523–1923 K. Oxidation with CO2 and H2O is not as thermodynamically favorable and largely dependent upon the oxidant concentration. The model is experimentally validated by O2 non-stoichiometry measurements at high temperatures (>1623 K) and CO2 reduction cycles with commercially available LSM35. Theoretical solar–fuel energy conversion efficiencies for LSM40 and ceria redox cycles are 16 and 22% at 1800 K and 13 and 7% at 1600 K, respectively.