Site-Selective Polyolefin Hydrogenolysis on Atomic Ru for Methanation Suppression and Liquid Fuel Production

Mingyu Chu; Xianpeng Wang; Xuchun Wang; Xiangxi Lou; Congyang Zhang; Muhan Cao; Lu Wang; Youyong Li; Sibao Liu; Tsun-Kong Sham; Qiao Zhang; Jinxing Chen

doi:10.34133/research.0032

Site-Selective Polyolefin Hydrogenolysis on Atomic Ru for Methanation Suppression and Liquid Fuel Production

Research (Wash D C). 2023:6:0032. doi: 10.34133/research.0032. Epub 2023 Jan 13.

Authors

Mingyu Chu¹, Xianpeng Wang¹, Xuchun Wang^{1

2}, Xiangxi Lou^{1

3}, Congyang Zhang^{1

2}, Muhan Cao¹, Lu Wang¹, Youyong Li¹, Sibao Liu⁴, Tsun-Kong Sham², Qiao Zhang¹, Jinxing Chen¹

Affiliations

¹ Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou 215123, P. R. China.
² Department of Chemistry, University of Western Ontario, London, Ontario N6A 5B7, Canada.
³ Key Laboratory of Superlight Materials and Surface Technology, Ministry of Education, College of Material Science and Chemical Engineering, Harbin Engineering University, Harbin 150001, China.
⁴ Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China.

Abstract

Catalytic hydrogenolysis of end-of-life polyolefins can produce value-added liquid fuels and therefore holds great promises in plastic waste reuse and environmental remediation. The major challenge limiting the recycling economic benefit is the severe methanation (usually >20%) induced by terminal C-C cleavage and fragmentation in polyolefin chains. Here, we overcome this challenge by demonstrating that Ru single-atom catalyst can effectively suppress methanation by inhibiting terminal C-C cleavage and preventing chain fragmentation that typically occurs on multi-Ru sites. The Ru single-atom catalyst supported on CeO₂ shows an ultralow CH₄ yield of 2.2% and a liquid fuel yield of over 94.5% with a production rate of 314.93 g_fuels g_Ru ^-1 h^-1 at 250 °C for 6 h. Such remarkable catalytic activity and selectivity of Ru single-atom catalyst in polyolefin hydrogenolysis offer immense opportunities for plastic upcycling.