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Bifunctional tandem catalytic upcycling of polyethylene to surfactant-range alkylaromatics
Chem ( IF 19.1 ) Pub Date : 2023-06-07 , DOI: 10.1016/j.chempr.2023.05.017
Jiakai Sun , Yu-Hsuan Lee , Ryan D. Yappert , Anne M. LaPointe , Geoffrey W. Coates , Baron Peters , Mahdi M. Abu-Omar , Susannah L. Scott

Catalytic conversion of waste polyolefins to value-added alkylaromatics could contribute to carbon recycling. Compared with tandem hydrogenolysis/aromatization of polyethylene (PE) catalyzed by Pt/γ-Al2O3 at 280°C, both a 5-fold enhancement in the rate of C–C bond scission and a doubling of the molar yield of alkylaromatics were achieved using a more acidic Pt/F-Al2O3 catalyst instead. Bifunctional (metal/acid) catalysts also generate alkylaromatic products with lower average carbon numbers (ca. C20), similar to conventional anionic surfactants. Because physical mixtures of weakly acidic Pt/γ-Al2O3 or non-acidic Pt/SiO2 with strongly Brønsted acidic Cl-Al2O3 or F-Al2O3 are also effective, the tandem reaction does not require nanoscale intimacy between metal and acid active sites. Kinetic studies using triacontane (norm-C30H62) as a model for PE show that the Pt-catalyzed dehydrogenation/hydrogenation reactions are quasi-equilibrated, while the acid-catalyzed C–C bond scission and skeletal transformations (isomerization and cyclization) determine the overall rates of depolymerization and aromatic formation.



中文翻译:

聚乙烯双功能串联催化升级循环为表面活性剂范围的烷基芳烃

将废弃聚烯烃催化转化为增值烷基芳烃可能有助于碳回收。与Pt/γ-Al 2 O 3在280℃催化聚乙烯(PE)串联氢解/芳构化相比,C-C键断裂速率提高了5倍,烷基芳烃摩尔产率提高了一倍使用酸性更强的 Pt/F-Al 2 O 3催化剂代替来实现。双功能(金属/酸)催化剂还可生成平均碳数较低(约 C 20 )的烷基芳族产物,与传统阴离子表面活性剂类似。因为弱酸性Pt/γ-Al 2 O 3或非酸性Pt/SiO 2的物理混合物具有强布朗斯台德酸性的Cl-Al 2 O 3或F-Al 2 O 3也有效,串联反应不需要金属和酸活性位点之间的纳米级紧密接触。使用三十烷( norm -C 30 H 62 )作为 PE 模型的动力学研究表明,Pt 催化的脱氢/氢化反应是准平衡的,而酸催化的 C-C 键断裂和骨架转化(异构化和环化确定解聚和芳香族形成的总体速率。

更新日期:2023-06-07
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