Angew. Chem. Int. Ed.: Entropy Confinement Promotes Hydrogenolysis Activity for Polyethylene Upcycling

Title：

Entropy Confinement Promotes Hydrogenolysis Activity for Polyethylene Upcycling

Authors：

Qingyun Kang^1#, Mingyu Chu^1,2#, Panpan Xu³, Xuchun Wang^1,4, Shiqi Wang⁵, Muhan Cao¹, Oleksandr Ivasenko¹, Tsun-Kong Sham⁴, Qiao Zhang¹, Qiming Sun⁵*, Jinxing Chen¹*

Institutions：

¹Institute of Functional Nano & Soft Materials (FUNSOM), Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices

²Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University, Suzhou 215123, P. R. China

³Key Laboratory of Multifunctional Nanomaterials and Smart Systems, Advanced Materials Division, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences Suzhou 215123, China

⁴Department of Chemistry University of Western Ontario London, Ontario, N6A 5B7, Canada

⁵Innovation Center for Chemical Sciences, College of Chemistry, Chemical Engineering and Materials Science Soochow University Suzhou 215123, P. R. China

Abstract：

Chemical upcycling that catalyzes waste plastics back to high-purity chemicals holds great promise in end-of-life plastics valorization. One of the main challenges in this process is the thermodynamic limitations imposed by the high intrinsic entropy of polymer chains, which makes their adsorption on catalysts unfavorable and the transition state unstable. Here, we overcome this challenge by inducing the catalytic reaction inside mesoporous channels, which possess a strong confined ability to polymer chains, allowing for stabilizing transition state. This approach involves the synthesis of p-Ru/SBA catalysts, in which Ru nanoparticles are uniformly distributed within the channels of an SBA-15 support, using a precise impregnation method. The unique design of the p-Ru/SBA catalyst has demonstrated significant improvements in catalytic performance for the conversion of polyethylene into high-valued liquid fuels, particularly diesel. The catalyst achieved a high solid conversion rate of 1106 g·g_Ru^-1·h^-1 at 230 °C. Comparatively, this catalytic activity is 4.9 times higher than that of a control catalyst, Ru/SiO₂, and 14.0 times higher than that of a commercial catalyst, Ru/C, at 240 °C. This remarkable catalytic activity opens up immense opportunities for the chemical upcycling of waste plastics.

IF：

16.823

Link：

https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202313174