Liu Yanchao, Dai Weijiong, Zheng Jiajun, Du Yanze, Wang Quanhua, Hedin Niklas, Qin Bo, Li Ruifeng
Research Centre of Energy Chemical & Catalytic Technology, Taiyuan University of Technology, Taiyuan, 030024, China.
SINOPEC Dalian Research Institute of Petroleum & Petrochemicals Co., Ltd, Dalian, 116045, China.
Adv Sci (Weinh). 2024 Sep;11(34):e2404426. doi: 10.1002/advs.202404426. Epub 2024 Jul 8.
Waste plastics bring about increasingly serious environmental challenges, which can be partly addressed by their interconversion into valuable compounds. It is hypothesized that the porosity and acidity of a zeolite-based catalyst will affect the selectivity and effectiveness, enabling a controllable and selective conversion of polyethylene (PE) into gas-diesel or lubricating base oil. A series of embryonic, partial- and well-crystalline zeolites beta with adjustable porosity and acidity are prepared from mesoporous SBA-15. The catalysts and catalytic systems are studied with nuclear magnetic resonance (NMR), X-ray diffraction (XRD), and adsorption kinetics and catalytic reactions. The adjustable porosity and acidity of zeolite-beta-based catalysts achieve a controllable selectivity toward gas-diesel or lubricating base oil for PE cracking. With a catalyst with mesopores and appropriate acid sites, a fast escape and reduced production of cracking of intermediates are observed, leading to a significant fraction (88.7%) of lubricating base oil. With more micropores, a high acid density, and strong acid strength, PE is multiply cracked into low carbon number hydrocarbons. The strong acid center of the zeolite is confirmed to facilitate significantly the activation of hydrogen (H), and, an in situ ammonia poisoning strategy can significantly inhibit hydrogen transfer and effectively regulate the product distribution.
废塑料带来了日益严峻的环境挑战,而将其转化为有价值的化合物可在一定程度上应对这些挑战。据推测,沸石基催化剂的孔隙率和酸度会影响选择性和效果,从而实现将聚乙烯(PE)可控且选择性地转化为气体柴油或润滑基础油。由介孔SBA - 15制备了一系列具有可调孔隙率和酸度的胚胎型、部分结晶型和结晶良好的β沸石。采用核磁共振(NMR)、X射线衍射(XRD)以及吸附动力学和催化反应对催化剂及催化体系进行了研究。基于β沸石的催化剂可调的孔隙率和酸度实现了对PE裂解生成气体柴油或润滑基础油的可控选择性。使用具有介孔和适当酸位点的催化剂时,观察到中间体快速逸出且裂解产物减少,从而得到很大比例(88.7%)的润滑基础油。当具有更多微孔、高酸密度和强酸强度时,PE会多次裂解为低碳数烃类。证实沸石的强酸中心能显著促进氢(H)的活化,并且,原位氨中毒策略可显著抑制氢转移并有效调节产物分布。