Yuan Yong, Xie Zhenhua, Turaczy Kevin K, Hwang Sooyeon, Zhou Jiahua, Chen Jingguang G
Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States.
Department of Chemical Engineering, Columbia University, New York, New York 10027, United States.
Chem Bio Eng. 2024 Jan 4;1(1):67-75. doi: 10.1021/cbe.3c00007. eCollection 2024 Feb 22.
Plastic hydrogenolysis is an attractive approach for producing value-added chemicals due to its mild reaction conditions, but controlling product distribution is challenging due to the formation of undesired CH This work reports several bimetallic RuM/CeO (M = Fe, Co, Ni) catalysts that shift the product of low-density polyethylene hydrogenolysis toward longer-chain hydrocarbons. These catalysts were characterized by using X-ray absorption fine structure spectroscopy, electron microscopy imaging, and H temperature-programmed reduction. The combined catalytic evaluation and characterization results revealed that the product distribution was regulated by the formation of bimetallic alloys. A model compound, -hexadecane, was selected to further understand the differences in hydrogenolysis over the Ru-based catalysts. Although a longer reaction time shifted the product toward smaller molecules, the bimetallic (RuCo/CeO) catalyst limited the further conversion of C2-C5 into CH. This work highlights the role of bimetallic alloys in tailoring the interaction with hydrocarbons, thereby controlling the product distribution of polymer hydrogenolysis.
由于反应条件温和，塑料氢解是一种生产增值化学品的有吸引力的方法，但由于会形成不希望的CH，控制产物分布具有挑战性。这项工作报道了几种双金属RuM/CeO（M = Fe、Co、Ni）催化剂，它们能使低密度聚乙烯氢解产物向长链烃类转变。通过使用X射线吸收精细结构光谱、电子显微镜成像和H程序升温还原对这些催化剂进行了表征。综合催化评价和表征结果表明，产物分布受双金属合金形成的调节。选择模型化合物正十六烷以进一步了解基于Ru的催化剂在氢解方面的差异。尽管较长的反应时间会使产物向小分子转变，但双金属（RuCo/CeO）催化剂限制了C2-C5进一步转化为CH。这项工作突出了双金属合金在调整与烃类相互作用从而控制聚合物氢解产物分布方面的作用。
