PMID- 38105396 OWN - NLM STAT- PubMed-not-MEDLINE LR - 20240304 IS - 1521-3773 (Electronic) IS - 1433-7851 (Linking) VI - 63 IP - 11 DP - 2024 Mar 11 TI - Consumer Grade Polyethylene Recycling via Hydrogenolysis on Ultrafine Supported Ruthenium Nanoparticles. PG - e202317526 LID - 10.1002/anie.202317526 [doi] AB - Catalytic hydrogenolysis has the potential to convert high-density polyethylene (HDPE), which comprises about 30 % of plastic waste, into valuable alkanes. Most investigations have focused on increasing activity for lab grade HDPEs displaying low molecular weight, with limited mechanistic understanding of the product distribution. No efficient catalyst is available for consumer grades due to their lower reactivity. This study targets HDPE used in bottle caps, a waste form generated globally at a rate of approximately one million units per hour. Ultrafine ruthenium particles (1 nm) supported on titania (anatase) achieved up to 80 % conversion into light alkanes (C(1) -C(45) ) under mild conditions (498 K, 20 bar H(2) , 4 h) and were reused for three cycles. Small ruthenium nanoparticles were critical to achieving relevant conversions, as activity sharply decreased with particle size. Selectivity commonalities and peculiarities across HDPE grades were disclosed by a reaction modelling approach applied to products. Isomerization cedes to backbone scission as the reaction progresses. Within this trend, low molecular weight favor isomerization whilst high molecular weight favor cleavage. Commercial caps obeyed this trend with decreased activity, anticipating the influence of additives in realistic processing. This study demonstrates effective hydrogenolysis of consumer grade polyethylene and provides selectivity patterns for product control. CI - (c) 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH. FAU - Jaydev, Shibashish D AU - Jaydev SD AUID- ORCID: 0000-0002-7251-273X AD - Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland. FAU - Martin, Antonio J AU - Martin AJ AUID- ORCID: 0000-0003-3482-8829 AD - Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland. FAU - Usteri, Marc-Eduard AU - Usteri ME AUID- ORCID: 0000-0002-9874-2736 AD - Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland. FAU - Chikri, Katia AU - Chikri K AD - Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland. FAU - Eliasson, Henrik AU - Eliasson H AUID- ORCID: 0000-0003-2975-0334 AD - Electron Microscopy Center, Swiss Federal Laboratories for Materials Science and Technology, Uberlandstrasse 129, 8600, Dubendorf, Switzerland. FAU - Erni, Rolf AU - Erni R AUID- ORCID: 0000-0003-2391-5943 AD - Electron Microscopy Center, Swiss Federal Laboratories for Materials Science and Technology, Uberlandstrasse 129, 8600, Dubendorf, Switzerland. FAU - Perez-Ramirez, Javier AU - Perez-Ramirez J AUID- ORCID: 0000-0002-5805-7355 AD - Institute of Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, Vladimir-Prelog-Weg 1, 8093, Zurich, Switzerland. LA - eng GR - ETH-40 20-2/Eidgenossische Technische Hochschule Zurich/ GR - 180544/NCCR Catalysis/ PT - Journal Article DEP - 20231228 PL - Germany TA - Angew Chem Int Ed Engl JT - Angewandte Chemie (International ed. in English) JID - 0370543 SB - IM OTO - NOTNLM OT - Chemical Plastic Recycling OT - Heterogenous Catalysis OT - Polyethylene Hydrogenolysis OT - Ruthenium Nanoparticles OT - Selectivity EDAT- 2023/12/18 00:42 MHDA- 2023/12/18 00:43 CRDT- 2023/12/17 23:52 PHST- 2023/11/17 00:00 [received] PHST- 2023/12/18 00:43 [medline] PHST- 2023/12/18 00:42 [pubmed] PHST- 2023/12/17 23:52 [entrez] AID - 10.1002/anie.202317526 [doi] PST - ppublish SO - Angew Chem Int Ed Engl. 2024 Mar 11;63(11):e202317526. doi: 10.1002/anie.202317526. Epub 2023 Dec 28.