Efficient solvent- and hydrogen-free upcycling of high-density polyethylene into separable cyclic hydrocarbons
Plastic pollution is a planetary threat that has been exacerbated by the COVID-19 pandemic due to the surge in medical waste, personal protective equipment and takeaway packaging. A socially sustainable and economically viable method for plastic recycling should not use consumable materials such as...
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| Veröffentlicht in: | Nature nanotechnology 2023-07, Vol.18 (7), p.772-779 |
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| creator | Du, Junjie Zeng, Lin Yan, Tao Wang, Chuanhao Wang, Menglin Luo, Lei Wu, Wenlong Peng, Zijun Li, Hongliang Zeng, Jie |
| description | Plastic pollution is a planetary threat that has been exacerbated by the COVID-19 pandemic due to the surge in medical waste, personal protective equipment and takeaway packaging. A socially sustainable and economically viable method for plastic recycling should not use consumable materials such as co-reactants or solvents. Here we report that Ru nanoparticles on zeolitic HZSM-5 catalyse the solvent- and hydrogen-free upcycling of high-density polyethylene into a separable distribution of linear (C
1
to C
6
) and cyclic (C
7
to C
15
) hydrocarbons. The valuable monocyclic hydrocarbons accounted for 60.3 mol% of the total yield. Based on mechanistic studies, the dehydrogenation of polymer chains to form C=C bonds occurs on both Ru sites and acid sites in HZSM-5, whereas carbenium ions are generated on the acid sites via the protonation of the C=C bonds. Accordingly, optimizing the Ru and acid sites promoted the cyclization process, which requires the simultaneous existence of a C=C bond and a carbenium ion on a molecular chain at an appropriate distance, providing high activity and cyclic hydrocarbon selectivity.
Ru nanoparticles on HZSM-5 catalysed solvent- and hydrogen-free upcycling of high-density polyethylene into a separable distribution of linear (C
1
to C
6
) and cyclic (C
7
to C
15
) hydrocarbons. |
| doi_str_mv | 10.1038/s41565-023-01429-9 |
| format | Article |
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1
to C
6
) and cyclic (C
7
to C
15
) hydrocarbons. The valuable monocyclic hydrocarbons accounted for 60.3 mol% of the total yield. Based on mechanistic studies, the dehydrogenation of polymer chains to form C=C bonds occurs on both Ru sites and acid sites in HZSM-5, whereas carbenium ions are generated on the acid sites via the protonation of the C=C bonds. Accordingly, optimizing the Ru and acid sites promoted the cyclization process, which requires the simultaneous existence of a C=C bond and a carbenium ion on a molecular chain at an appropriate distance, providing high activity and cyclic hydrocarbon selectivity.
Ru nanoparticles on HZSM-5 catalysed solvent- and hydrogen-free upcycling of high-density polyethylene into a separable distribution of linear (C
1
to C
6
) and cyclic (C
7
to C
15
) hydrocarbons.</description><identifier>ISSN: 1748-3387</identifier><identifier>EISSN: 1748-3395</identifier><identifier>DOI: 10.1038/s41565-023-01429-9</identifier><identifier>PMID: 37365277</identifier><language>eng</language><publisher>London: Nature Publishing Group UK</publisher><subject>140/131 ; 140/146 ; 639/638/77/887 ; 639/925/357/354 ; Chemistry and Materials Science ; COVID-19 ; Cyclic hydrocarbons ; Dehydrogenation ; High density polyethylenes ; Hydrocarbons ; Hydrogen ; Materials Science ; Medical equipment ; Medical wastes ; Molecular chains ; Nanoparticles ; Nanotechnology ; Nanotechnology and Microengineering ; Pandemics ; Plastic pollution ; Plastics recycling ; Polyethylene ; Polymers ; Protective equipment ; Protonation ; Ruthenium ; Solvents</subject><ispartof>Nature nanotechnology, 2023-07, Vol.18 (7), p.772-779</ispartof><rights>The Author(s), under exclusive licence to Springer Nature Limited 2023. Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.</rights><rights>2023. The Author(s), under exclusive licence to Springer Nature Limited.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c375t-1f0cdb956d1e6638cbe0b725809f795b75128fc081e0e7ddade17e5d4405a6083</citedby><cites>FETCH-LOGICAL-c375t-1f0cdb956d1e6638cbe0b725809f795b75128fc081e0e7ddade17e5d4405a6083</cites><orcidid>0009-0009-6918-231X ; 0000-0001-5440-2070 ; 0009-0002-8487-8357 ; 0000-0003-0134-5935 ; 0009-0000-3203-8706 ; 0000-0002-0793-6763 ; 0000-0003-0348-7910 ; 0000-0002-8812-0298</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/37365277$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Du, Junjie</creatorcontrib><creatorcontrib>Zeng, Lin</creatorcontrib><creatorcontrib>Yan, Tao</creatorcontrib><creatorcontrib>Wang, Chuanhao</creatorcontrib><creatorcontrib>Wang, Menglin</creatorcontrib><creatorcontrib>Luo, Lei</creatorcontrib><creatorcontrib>Wu, Wenlong</creatorcontrib><creatorcontrib>Peng, Zijun</creatorcontrib><creatorcontrib>Li, Hongliang</creatorcontrib><creatorcontrib>Zeng, Jie</creatorcontrib><title>Efficient solvent- and hydrogen-free upcycling of high-density polyethylene into separable cyclic hydrocarbons</title><title>Nature nanotechnology</title><addtitle>Nat. Nanotechnol</addtitle><addtitle>Nat Nanotechnol</addtitle><description>Plastic pollution is a planetary threat that has been exacerbated by the COVID-19 pandemic due to the surge in medical waste, personal protective equipment and takeaway packaging. A socially sustainable and economically viable method for plastic recycling should not use consumable materials such as co-reactants or solvents. Here we report that Ru nanoparticles on zeolitic HZSM-5 catalyse the solvent- and hydrogen-free upcycling of high-density polyethylene into a separable distribution of linear (C
1
to C
6
) and cyclic (C
7
to C
15
) hydrocarbons. The valuable monocyclic hydrocarbons accounted for 60.3 mol% of the total yield. Based on mechanistic studies, the dehydrogenation of polymer chains to form C=C bonds occurs on both Ru sites and acid sites in HZSM-5, whereas carbenium ions are generated on the acid sites via the protonation of the C=C bonds. Accordingly, optimizing the Ru and acid sites promoted the cyclization process, which requires the simultaneous existence of a C=C bond and a carbenium ion on a molecular chain at an appropriate distance, providing high activity and cyclic hydrocarbon selectivity.
Ru nanoparticles on HZSM-5 catalysed solvent- and hydrogen-free upcycling of high-density polyethylene into a separable distribution of linear (C
1
to C
6
) and cyclic (C
7
to C
15
) hydrocarbons.</description><subject>140/131</subject><subject>140/146</subject><subject>639/638/77/887</subject><subject>639/925/357/354</subject><subject>Chemistry and Materials Science</subject><subject>COVID-19</subject><subject>Cyclic hydrocarbons</subject><subject>Dehydrogenation</subject><subject>High density polyethylenes</subject><subject>Hydrocarbons</subject><subject>Hydrogen</subject><subject>Materials Science</subject><subject>Medical equipment</subject><subject>Medical wastes</subject><subject>Molecular chains</subject><subject>Nanoparticles</subject><subject>Nanotechnology</subject><subject>Nanotechnology and Microengineering</subject><subject>Pandemics</subject><subject>Plastic pollution</subject><subject>Plastics recycling</subject><subject>Polyethylene</subject><subject>Polymers</subject><subject>Protective 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Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Du, Junjie</au><au>Zeng, Lin</au><au>Yan, Tao</au><au>Wang, Chuanhao</au><au>Wang, Menglin</au><au>Luo, Lei</au><au>Wu, Wenlong</au><au>Peng, Zijun</au><au>Li, Hongliang</au><au>Zeng, Jie</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Efficient solvent- and hydrogen-free upcycling of high-density polyethylene into separable cyclic hydrocarbons</atitle><jtitle>Nature nanotechnology</jtitle><stitle>Nat. Nanotechnol</stitle><addtitle>Nat Nanotechnol</addtitle><date>2023-07-01</date><risdate>2023</risdate><volume>18</volume><issue>7</issue><spage>772</spage><epage>779</epage><pages>772-779</pages><issn>1748-3387</issn><eissn>1748-3395</eissn><abstract>Plastic pollution is a planetary threat that has been exacerbated by the COVID-19 pandemic due to the surge in medical waste, personal protective equipment and takeaway packaging. A socially sustainable and economically viable method for plastic recycling should not use consumable materials such as co-reactants or solvents. Here we report that Ru nanoparticles on zeolitic HZSM-5 catalyse the solvent- and hydrogen-free upcycling of high-density polyethylene into a separable distribution of linear (C
1
to C
6
) and cyclic (C
7
to C
15
) hydrocarbons. The valuable monocyclic hydrocarbons accounted for 60.3 mol% of the total yield. Based on mechanistic studies, the dehydrogenation of polymer chains to form C=C bonds occurs on both Ru sites and acid sites in HZSM-5, whereas carbenium ions are generated on the acid sites via the protonation of the C=C bonds. Accordingly, optimizing the Ru and acid sites promoted the cyclization process, which requires the simultaneous existence of a C=C bond and a carbenium ion on a molecular chain at an appropriate distance, providing high activity and cyclic hydrocarbon selectivity.
Ru nanoparticles on HZSM-5 catalysed solvent- and hydrogen-free upcycling of high-density polyethylene into a separable distribution of linear (C
1
to C
6
) and cyclic (C
7
to C
15
) hydrocarbons.</abstract><cop>London</cop><pub>Nature Publishing Group UK</pub><pmid>37365277</pmid><doi>10.1038/s41565-023-01429-9</doi><tpages>8</tpages><orcidid>https://orcid.org/0009-0009-6918-231X</orcidid><orcidid>https://orcid.org/0000-0001-5440-2070</orcidid><orcidid>https://orcid.org/0009-0002-8487-8357</orcidid><orcidid>https://orcid.org/0000-0003-0134-5935</orcidid><orcidid>https://orcid.org/0009-0000-3203-8706</orcidid><orcidid>https://orcid.org/0000-0002-0793-6763</orcidid><orcidid>https://orcid.org/0000-0003-0348-7910</orcidid><orcidid>https://orcid.org/0000-0002-8812-0298</orcidid></addata></record> |
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| source | Nature; Alma/SFX Local Collection |
| subjects | 140/131 140/146 639/638/77/887 639/925/357/354 Chemistry and Materials Science COVID-19 Cyclic hydrocarbons Dehydrogenation High density polyethylenes Hydrocarbons Hydrogen Materials Science Medical equipment Medical wastes Molecular chains Nanoparticles Nanotechnology Nanotechnology and Microengineering Pandemics Plastic pollution Plastics recycling Polyethylene Polymers Protective equipment Protonation Ruthenium Solvents |
| title | Efficient solvent- and hydrogen-free upcycling of high-density polyethylene into separable cyclic hydrocarbons |
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