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用于可持续生产丙烯醛的分级多孔钙钛矿催化剂上生物醇混合物的氧化偶联反应

Oxidative coupling of bio-alcohols mixture over hierarchically porous perovskite catalysts for sustainable acrolein production.

作者信息

Essehaity Al-Shaimaa M, Abd ElHafiz Dalia R, Aman Delvin, Mikhail Sara, Abdel-Monem Yasser K

机构信息

Catalysis Laboratory, Refining Department, Egyptian Petroleum Research Institute (EPRI) Nasr City 11727 Cairo Egypt

EPRI-Nanotechnology Center, Egyptian Petroleum Research Institute (EPRI) Nasr City 11727 Cairo Egypt.

出版信息

RSC Adv. 2021 Aug 31;11(46):28961-28972. doi: 10.1039/d1ra05627a. eCollection 2021 Aug 23.

Abstract

The acrolein production from bio-alcohols methanol and ethanol mixtures using AMnO (since A = Ba and/or Sr) perovskite catalysts was studied. All the prepared samples were characterized by XRD, XPS, N sorption, FTIR, Raman spectroscopy, TEM, SEM, TGA, and NH-CO-TPD. The catalytic oxidation reaction to produce acrolein has occurred two steps, the alcohols are firstly oxidized to corresponding aldehydes, and then the aldol is coupled with the produced aldehydes. The prepared perovskite samples were modified by doping A (Sr) position with (Ba) to improve the aldol condensation. The most catalytic performance was achieved using the BaSrMnO sample in which the acrolein selectivity reached 62% ( = 300 °C, MetOH/EtOH = 1, LHSV = 10 h). The increase in acrolein production may be related to the high tendency of BaSrMnO toward C-C coupling formation. The C-C tendency attributes to that modification have occurred in acid/base sites because of metal substitution.

摘要

研究了使用AMnO(其中A = Ba和/或Sr)钙钛矿催化剂由生物醇甲醇和乙醇混合物生产丙烯醛的过程。所有制备的样品均通过XRD、XPS、N吸附、FTIR、拉曼光谱、TEM、SEM、TGA和NH-CO-TPD进行表征。生产丙烯醛的催化氧化反应分两步进行,醇首先被氧化为相应的醛,然后醛醇与生成的醛偶联。通过用(Ba)掺杂A(Sr)位来改性制备的钙钛矿样品,以改善醛醇缩合反应。使用BaSrMnO样品获得了最佳催化性能,其中丙烯醛选择性在300℃、甲醇/乙醇=1、LHSV = 10 h-1的条件下达到62%。丙烯醛产量的增加可能与BaSrMnO对C-C偶联形成的高倾向有关。C-C倾向归因于由于金属取代而在酸/碱位点发生了改性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2861/9038184/7e3380070a23/d1ra05627a-f1.jpg

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