题目： | Stable Interfacial Ruthenium Species for Highly Efficient Polyolefin Upcycling |
作者： | Ping Hu1,2#, Congyang Zhang1,3#, Mingyu Chu1,2#, Xianpeng Wang1,4#, Lu Wang1,2, Youyong Li1,2,4, Tianran Yan1,2, Liang Zhang1,2, Zhifeng Ding3, Muhan Cao1,5, Panpan Xu6, Yifan Li6, Yi Cui6, Qiao Zhang1, Jinxing Chen1,2*, Lifeng Chi1,2,4* |
单位： | 1Institute of Functional Nano & Soft Materials (FUNSOM), Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou 215123, P. R. China 2Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, P. R. China 3Department of Chemistry, University of Western Ontario, London N6A 5B7, Canada 4Macao Institute of Materials Science and Engineering, Macau University of Science and Technology, Macau 999078, P. R. China 5Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou 215123, P. R. China 6Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou 215123, P. R. China |
摘要： | The present polyolefin hydrogenolysis recycling cases acknowledge that zerovalent Ru exhibits high catalytic activity. A pivotal rationale behind this assertion lies in the propensity of the majority of Ru species to undergo reduction to zerovalent Ru within the hydrogenolysis milieu. Nonetheless, the suitability of zerovalent Ru as an optimal structural configuration for accommodating multiple elementary reactions remains ambiguous. Here, we have constructed stable Ru0–Ruδ+ complex species, even under reaction conditions, through surface ligand engineering of commercially available Ru/C catalysts. Our findings unequivocally demonstrate that surface-ligated Ru species can be stabilized in the form of a Ruδ+ state, which, in turn, engenders a perturbation of the σ bond electron distribution within the polyolefin carbon chain, ultimately boosting the rate-determining step of C–C scission. The optimized catalysts reach a solid conversion rate of 609 g·gRu–1·h–1 for polyethylene. This achievement represents a 4.18-fold enhancement relative to the pristine Ru/C catalyst while concurrently preserving a remarkable 94% selectivity toward valued liquid alkanes. Of utmost significance, this surface ligand engineering can be extended to the gentle mixing of catalysts in ligand solution at room temperature, thus rendering it amenable for swift integration into industrial processes involving polyolefin degradation. |
影响因子： | 16.383 |
分区情况： | 一区 |
链接： |
责任编辑：郭佳