Vapor-phase conversion of aqueous 3-hydroxybutyric acid and crotonic acid to propylene over solid acid catalysts

Vapor-phase conversion of aqueous 3-hydroxybutyric acid and crotonic acid to propylene over solid acid catalysts
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固体酸催化剂上水性 3-羟基丁酸和巴豆酸气相转化为丙烯

DOI:
10.1039/d1cy01152a
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发表时间:
2021
影响因子:
5
通讯作者:
Strathmann, Timothy J.
Strathmann, Timothy J.
中科院分区:
化学2区
文献类型:
--
作者:
Leow, Shijie;Koehler, Andrew J.;Cronmiller, Lauren E.;Huo, Xiangchen;Lahti, Gabriella D.;Li, Yalin;Hafenstine, Glenn R.;Vardon, Derek R.;Strathmann, Timothy J.

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不同来源的废水有机碳可以微生物转化为聚羟基丁酸酯(PHB)等生物聚合物,通过转化为碳氢燃料和工业化学品进一步进行定价。报道了在填充床连续流动反应器中,PHB衍生的单体酸3-羟基丁酸(3HB)和巴豆酸(CA)在固体酸催化剂上的气相脱水和脱羧制丙烯。丙烯的产率随着催化剂的Brnsted酸度的增加而增加,无定形硅铝和磷酸Nb分别获得原料3HB和CA的52%和60%(原料碳百分比,最大75%C);额外的产物包括二氧化碳和复古-羟醛产物(乙醛和醋酸)。失活研究表明,无定形硅铝的水蒸气失活是渐进的和永久的,而再焙烧部分恢复了磷酸铌的活性。实验证明,磷酸铌反应器的持续运行为提高有机废水的价态提供了一条有希望的技术途径。
Diverse sources of wastewater organic carbon can be microbially funneled into biopolymers like polyhydroxybutyrate (PHB) that can be further valorized by conversion to hydrocarbon fuels and industrial chemicals. We report the vapor-phase dehydration and decarboxylation of PHB-derived monomer acids, 3-hydroxybutyric acid (3HB) and crotonic acid (CA), in water to propylene over solid acid catalysts using a packed-bed continuous-flow reactor. Propylene yields increase with increased Brønsted acidity of catalysts, with amorphous silica–alumina and niobium phosphate yielding 52 and 60 %C (percent feedstock carbon, max 75 %C) of feedstock 3HB and CA, respectively; additional products include CO2 and retro-aldol products (acetaldehyde and acetic acid). Deactivation studies indicate progressive and permanent steam deactivation of amorphous silica–alumina, while re-calcination partially recovers niobium phosphate activity. Experiments demonstrating sustained reactor operation over niobium phosphate provide a promising technology pathway for increasing valorization of organic-rich wastewater.
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