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Efficient and stable Fe-Ce-Al catalyst for catalytic deoxygenation of lignin for phenol and hydrocarbon-rich fuel: Effect of the synthesis method
Fuel Processing Technology ( IF 7.5 ) Pub Date : 2024-01-11 , DOI: 10.1016/j.fuproc.2024.108034
Yifei Chen , Hongyuan Wang , Jida Wang , Defa Hou , Yi Lu , Fulin Yang , Can Liu , Xu Lin , Zhifeng Zheng , Yunwu Zheng

To develop a structure-tailoring catalyst for catalytic conversion of lignin for value-added chemicals, a series of novel Fe-Ce-Al metal oxide catalysts was synthesized via different methods to tailor activity and structure for catalytic pyrolysis of lignin to enhance hydrocarbon-rich bio-oil. The results revealed that FeCeAl-CO catalysts derived from coprecipitation method with smaller particle sizes exhibited excellent catalytic deoxygenation activity due to higher Lewis/Brønsted acid, reversible Ce3+/Ce4+ redox pairs, tailorable oxygen vacancies and promoted β-O-4, aromatic-OCH3 and side-chain cleavage. Additionally, coprecipitation method was facilitated to enhance hydrogen transfer, side-chain cleavage and aromatization reactions, while wet impregnation was beneficial to enhance demethoxylation and H-abstraction activity. During catalytic pyrolysis process, over 57.91% of hydrocarbon, including 20.21% and 25.71% for aromatics and olefins were achieved over FeCeAl-CO catalyst. Over 60.74% phenols and 52.48% alkylphenols were obtained over Fe-Ce/Al2O3-IM catalyst due to synergistic effect of FeOx and CeOx species. Fe-Ce-Al catalyst exhibited great activity and stability after fourth run, greater Brønsted acid-favored lignin cleavage and coke deposition, and metal active species leaching, oxidation and pore blockage were the key reasons for deactivation. Therefore, these findings could provide a cost-effective method for designing structure-tailoring catalysts for direct catalytic deoxygenation of lignin to generate hydrocarbon-rich upgrading bio-oil.



中文翻译:

高效稳定的 Fe-Ce-Al 催化剂用于木质素催化脱氧生产苯酚和富烃燃料:合成方法的效果

为了开发用于木质素催化转化为增值化学品的结构定制催化剂,通过不同的方法合成了一系列新型Fe-Ce-Al金属氧化物催化剂,以定制木质素催化热解的活性和结构,以增强富烃能力生物油。结果表明,共沉淀法制备的具有较小粒径的FeCeAl-CO催化剂由于较高的Lewis/Brønsted酸、可逆的Ce 3+ /Ce 4+氧化还原对、可调节的氧空位和促进的β-O-4而表现出优异的催化脱氧活性。 、芳香族-OCH 3和侧链裂解。此外,共沉淀法有利于增强氢转移、侧链断裂和芳构化反应,而湿浸渍有利于增强脱甲氧基化和H-抽象活性。在催化热解过程中,在FeCeAl-CO催化剂上,烃类的产率超过57.91%,其中芳烃和烯烃的产率分别为20.21%和25.71%。由于FeOx和CeOx物质的协同作用,在Fe-Ce/Al 2 O 3 -IM催化剂上得到了超过60.74%的苯酚和52.48%的烷基酚。Fe-Ce-Al催化剂在第四次运行后表现出良好的活性和稳定性,较大的布朗斯台德酸有利于木质素裂解和积炭,金属活性物质的浸出、氧化和孔堵塞是失活的关键原因。因此,这些发现可以为设计结构定制催化剂提供一种经济有效的方法,用于木质素的直接催化脱氧以产生富含碳氢化合物的升级生物油。

更新日期:2024-01-15
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