Ultratough Thermoplastic Elastomers Based on Chemically Recyclable Cycloalkyl-Substituted Polyhydroxyalkanoates

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: 147(9), P. 7788 - 7798

Published: Feb. 20, 2025

It remains a long-standing challenge for chemical recycling of polyhydroxyalkanoates (PHAs) to propiolactone-based monomers due the high ring strain and many inevitable side reactions. In this contribution, novel α-spiro-cyclohexyl-propiolactone (SHPL) has been designed with reactivity toward ring-opening polymerization even at catalyst loading <1 ppm. The resulting poly(3-hydroxy-2-spiro-cyclohexylpropionate) (P3HSHP) exhibited thermal stability Td 364 °C Tm 272 °C. Meanwhile, it could be depolymerized back SHPL in 86% yield without decarboxylation or elimination products. Notably, exploited construct high-performance thermoplastic elastomers (TPEs) via one-pot copolymerization ε-caprolactone (CL). Particularly, gradient P(CL2000-grad-SHPL500) showcased an ultimate tensile strength 58.8 ± 4.0 MPa, stretchability 1959 53%, record toughness 600 MJ/m3, elastic recovery (>90%). This superior performance advance development new sustainable TPEs.

Language: Английский

---

Co-recycling of plastics and other waste materials

Published: April 28, 2025

Language: Английский

---

Micelles Cascade Assembly to Tandem Porous Catalyst for Waste Plastics Upcycling

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(26)

Published: April 22, 2024

Catalytic upcycling of polyolefins into high-value chemicals represents the direction in end-of-life plastics valorization, but poses great challenges. Here, we report synthesis a tandem porous catalyst via micelle cascade assembly strategy for selectively catalytic cracking polyethylene olefins at low temperature. A hierarchically silica layer from mesopore to macropore is constructed on surface microporous ZSM-5 nanosheets through dynamic micelles. The outer arrays can adsorb bulky quickly by capillary and hydrophobic effects, enhancing diffusion access active sites. middle mesopores present nanoconfinement space, pre-cracking intermediates weak acid sites, which then transport zeolites micropores further strong Brønsted acidic structures, mimicking biomimetic protease clefts, ideally match steps polyolefins, thus suppressing coke formation facilitating product escape. As result, light hydrocarbons (C

Language: Английский

---

Automated Ultra-Fast ¹³C NMR Analysis of Polyolefin Materials

Analytical Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 21, 2025

Polyolefins are unique among synthetic polymers because their wide application envelope originates from a finely controlled microstructure of hydrocarbon chains, lacking any distinctive functional groups. This hampers the methods automated sorting based on vibrational spectroscopies and calls for much more complex 13C NMR elucidations. High-temperature cryoprobes have dramatically shortened acquisition time spectra, few minutes now enough polyolefin classification purposes; however, conventional data analysis remains labor time-consuming. In this paper, we introduce an instrument fast determinations materials, implemented by integrating High-Throughput Experimentation Data Science tools methods. From scientific standpoint, main interest approach is solution proposed to address general problem how rapidly characterize statistically distributed analytes, which most important case. practical terms, represents first tool microstructural analysis: it readily applicable monomaterials, whereas extension multimaterials, including postconsumer streams, feasible but still requires some work.

Language: Английский

---

Comparison of Computational Methods for Simulating Depolymerization Reaction

ACS Omega, Journal Year: 2025, Volume and Issue: 10(6), P. 5973 - 5980

Published: Feb. 4, 2025

A chemical recycling process that reduces polymers to their raw materials plays a crucial role in circular economy. To contribute recycling, this study proposes system simulates the of depolymerization from polymer-to-monomer using reactive molecular dynamics (MD). Two MD methods, Reax force field (ReaxFF) and neural network potential (NNP), were employed simulate polystyrene model. We validated simulation accuracies by comparing monomer yields decomposition products with experimental results. The results showed NNP-MD accurately replicated degradation redecomposition processes achieved consistency data at various temperatures. ReaxFF-MD, however, was less able represent process. conclude is capable simulating polymer are consistent observations. These development methods for efficient broader realization

Language: Английский

---

One-Pot Upcycling of Polycarbonate into BPA-Poly(ether-carbonate) Polyols for Polyurethane Applications

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 25, 2025

Language: Английский

---

Recycling Polyester and Polycarbonate Plastics with Carbocation Lewis Acidic Organocatalysts

ACS Macro Letters, Journal Year: 2025, Volume and Issue: unknown, P. 377 - 384

Published: March 8, 2025

The effective management of plastic waste is critical for environmental sustainability. This work explores the use carbocation catalysts recycling common polyesters and polycarbonates through alcoholysis. We demonstrate complete depolymerization end-of-life materials investigate relationship between catalytic reactivity structural features compounds, including cations their counteranions. Carbocations function as Lewis acids, facilitating interaction with carbonyls in polymer chains. Moreover, our approach enables hierarchical degradation polyester blends. research not only elucidates role carbocations alcoholysis these polymers, but also establishes a metal-free process efficient plastics.

Language: Английский

---

Upcycling waste commodity polymers into high-performance polyarylate materials with direct utilization of capping agent impurities

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: March 12, 2025

Commodity polymers are ubiquitous in our society, having replaced many inorganic and metal-based materials due to their versatile properties. However, functionality heavily relies on the addition of various components known as additives, making it challenging recycle polymer fraction plastic effectively. Thus, is crucial develop efficient chemical recovery strategies for commodity additives facilitate direct utilization recovered monomers without additional purification. Here, we a strategy co-upcycling two types waste polymers, polycarbonate, polyethylene terephthalate into polyarylate, high-performance transparent engineering plastic. By incorporating highly active metal-free ionic liquids catalyst methanolysis two-stage interface polymerization technique with variable temperature control, successfully prepare polyacrylate film from real end-of-life plastics capping agent impurities monomers. These exhibit excellent thermal performance (Tg = 192.8 °C), transmittance (reach up 86.73%), flame-retardant properties (V-0, UL-94), equivalent those commercial polyarylate (U-100, about $10000/ton), could be further easily close-loop recycled. Demonstrated kilogram-scale experiments life cycle assessments, this approach offers low-carbon, environmentally friendly, economically feasible pathway upcycling polymers. Recycling remains presence mixed streams. Here authors terephthalate,

Language: Английский

---

Global Trends and Strategic Pathways for Waste Plastics Depolymerization in the Circular Economy

Cleaner Waste Systems, Journal Year: 2025, Volume and Issue: unknown, P. 100292 - 100292

Published: April 1, 2025

Language: Английский

---

Exploring the Reaction Mechanism of Polyethylene Terephthalate Biodegradation through QM/MM Approach

The Journal of Physical Chemistry B, Journal Year: 2024, Volume and Issue: 128(31), P. 7486 - 7499

Published: July 29, 2024

The enzyme PETase from

Language: Английский

---