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无镧系元素钙钛矿氧化物催化剂用于通过氧化还原机制进行乙苯脱氢反应。

Lanthanoid-free perovskite oxide catalyst for dehydrogenation of ethylbenzene working with redox mechanism.

机构信息

Department of Materials Science and Chemical Engineering, Faculty of Engineering, Shizuoka University Hamamatsu, Japan.

Department of Applied Chemistry, School of Science and Engineering, Waseda University Tokyo, Japan.

出版信息

Front Chem. 2013 Oct 23;1:21. doi: 10.3389/fchem.2013.00021. eCollection 2013.

DOI:10.3389/fchem.2013.00021
PMID:24790949
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC3982525/
Abstract

For the development of highly active and robust catalysts for dehydrogenation of ethylbenzene (EBDH) to produce styrene; an important monomer for polystyrene production, perovskite-type oxides were applied to the reaction. Controlling the mobility of lattice oxygen by changing the structure of Ba1 - x SrxFe y Mn1 - y O3 - δ (0 ≤ x ≤ 1, 0.2 ≤ y ≤ 0.8), perovskite catalyst showed higher activity and stability on EBDH. The optimized Ba/Sr and Fe/Mn molar ratios were 0.4/0.6 and 0.6/0.4, respectively. Comparison of the dehydrogenation activity of Ba0.4Sr0.6Fe0.6Mn0.4O3 - δ catalyst with that of an industrial potassium promoted iron (Fe-K) catalyst revealed that the Ba0.4Sr0.6Fe0.6Mn0.4O3 - δ catalyst showed higher initial activity than the industrial Fe-K oxide catalyst. Additionally, the Ba0.4Sr0.6Fe0.6Mn0.4O3 - δ catalyst showed high activity and stability under severe conditions, even at temperatures as low as 783 K, or at the low steam/EB ratio of 2, while, the Fe-K catalyst showed low activity in such conditions. Comparing reduction profiles of the Ba0.4Sr0.6Fe0.6Mn0.4O3 - δ and the Fe-K catalysts in a H2O/H2 atmosphere, reduction was suppressed by the presence of H2O over the Ba0.4Sr0.6Fe0.6Mn0.4O3 - δ catalyst while the Fe-K catalyst was reduced. In other words, Ba0.4Sr0.6Fe0.6Mn0.4O3 - δ catalyst had higher potential for activating the steam than the Fe-K catalyst. The lattice oxygen in perovskite-structure was consumed by H2, subsequently the consumed lattice oxygen was regenerated by H2O. So the catalytic performance of Ba0.4Sr0.6Fe0.6Mn0.4O3 - δ was superior to that of Fe-K catalyst thanks to the high redox property of the Ba0.4Sr0.6Fe0.6Mn0.4O3 - δ perovskite oxide.

摘要

为了开发高效且稳定的乙基苯脱氢制苯乙烯催化剂，用于生产聚苯乙烯的重要单体；钙钛矿型氧化物被应用于该反应。通过改变 Ba1-xSrxFe y Mn1-yO3-δ（0≤x≤1，0.2≤y≤0.8）的结构来控制晶格氧的迁移率，钙钛矿型催化剂在乙基苯脱氢反应中表现出更高的活性和稳定性。优化的 Ba/Sr 和 Fe/Mn 摩尔比分别为 0.4/0.6 和 0.6/0.4。与工业钾促进铁（Fe-K）催化剂相比，Ba0.4Sr0.6Fe0.6Mn0.4O3-δ催化剂的脱氢活性表明，Ba0.4Sr0.6Fe0.6Mn0.4O3-δ催化剂的初始活性高于工业 Fe-K 氧化物催化剂。此外，Ba0.4Sr0.6Fe0.6Mn0.4O3-δ催化剂在苛刻条件下表现出高活性和稳定性，即使在 783 K 的低温或蒸汽/EB 比低至 2 的条件下，而 Fe-K 催化剂在这些条件下活性较低。在 H2O/H2 气氛中比较 Ba0.4Sr0.6Fe0.6Mn0.4O3-δ和 Fe-K 催化剂的还原曲线，Ba0.4Sr0.6Fe0.6Mn0.4O3-δ催化剂上存在 H2O 会抑制还原，而 Fe-K 催化剂则会被还原。换句话说，Ba0.4Sr0.6Fe0.6Mn0.4O3-δ催化剂比 Fe-K 催化剂更有潜力激活蒸汽。钙钛矿结构中的晶格氧被 H2 消耗，随后消耗的晶格氧被 H2O 再生。因此，Ba0.4Sr0.6Fe0.6Mn0.4O3-δ 催化剂的催化性能优于 Fe-K 催化剂，这要归功于 Ba0.4Sr0.6Fe0.6Mn0.4O3-δ 钙钛矿氧化物的高氧化还原性能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/4354c5179971/fchem-01-00021-g0009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/719c489a55ab/fchem-01-00021-g0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/cbe6c741e746/fchem-01-00021-g0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/2d79eb084288/fchem-01-00021-g0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/ad0ed4c1e557/fchem-01-00021-g0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/262794b4a9ee/fchem-01-00021-g0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/ef37fd5742b9/fchem-01-00021-g0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/f705912b4ece/fchem-01-00021-g0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/7e70689f7d43/fchem-01-00021-g0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/4354c5179971/fchem-01-00021-g0009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/719c489a55ab/fchem-01-00021-g0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/cbe6c741e746/fchem-01-00021-g0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/2d79eb084288/fchem-01-00021-g0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/ad0ed4c1e557/fchem-01-00021-g0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/262794b4a9ee/fchem-01-00021-g0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/ef37fd5742b9/fchem-01-00021-g0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/f705912b4ece/fchem-01-00021-g0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/7e70689f7d43/fchem-01-00021-g0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/be7c/3982525/4354c5179971/fchem-01-00021-g0009.jpg

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