Recyclable and (Bio)degradable Polyesters in a Circular Plastics Economy

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(7), P. 4393 - 4478

Published: March 22, 2024

Polyesters carrying polar main-chain ester linkages exhibit distinct material properties for diverse applications and thus play an important role in today's plastics economy. It is anticipated that they will even greater tomorrow's circular economy focuses on sustainability, thanks to the abundant availability of their biosourced building blocks presence bonds can be chemically or biologically cleaved demand by multiple methods bring about more desired end-of-life plastic waste management options. Because this potential promise, there have been intense research activities directed at addressing recycling, upcycling biodegradation existing legacy polyesters, designing biorenewable alternatives, redesigning future polyesters with intrinsic chemical recyclability tailored performance rival commodity are either petroleum based and/or hard recycle. This review captures these exciting recent developments outlines challenges opportunities. Case studies poly(lactic acid), poly(3-hydroxyalkanoate)s, poly(ethylene terephthalate), poly(butylene succinate), poly(butylene-adipate presented, emerging recyclable comprehensively reviewed.

Language: Английский

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Mixed Plastics Wastes Upcycling with High-Stability Single-Atom Ru Catalyst

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(41), P. 22836 - 22844

Published: Oct. 5, 2023

Mixed plastic waste treatment has long been a significant challenge due to complex composition and sorting costs. In this study, we have achieved breakthrough in converting mixed wastes into single chemical product using our innovative single-atom catalysts for the first time. The Ru catalyst can convert ∼90% of real methane products (selectivity >99%). unique electronic structure sites regulates adsorption energy intermediates, leading rapid decomposition plastics superior cycle stability compared traditional nanocatalysts. global warming potential entire process was evaluated. Our proposed carbon-reducing utilizing launches new era valorization.

Language: Английский

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New Advances in Covalent Network Polymers via Dynamic Covalent Chemistry

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(12), P. 7829 - 7906

Published: June 3, 2024

Covalent network polymers, as materials composed of atoms interconnected by covalent bonds in a continuous network, are known for their thermal and chemical stability. Over the past two decades, these have undergone significant transformations, gaining properties such malleability, environmental responsiveness, recyclability, crystallinity, customizable porosity, enabled development integration dynamic chemistry (DCvC). In this review, we explore innovative realm polymers focusing on recent advances achieved through application DCvC. We start examining history fundamental principles DCvC, detailing its inception core concepts noting key role reversible bond formation. Then reprocessability DCvC is thoroughly discussed, starting from milestones that marked evolution progressing to current trends applications. The influence crystallinity then reviewed, covering diversity, synthesis techniques, functionalities. concluding section, address challenges faced field speculates potential future directions.

Language: Английский

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Improving Charge Storage of Biaxially‐Oriented Polypropylene under Extreme Electric Fields by Excimer UV Irradiation

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Feb. 2, 2024

Abstract Biaxially‐oriented polypropylene (BOPP) is one of the most commonly used materials for film‐based capacitors power electronics and pulsed systems. To address pressing issue performance‐limiting loss under extreme electric‐fields, here a one‐step, high‐throughput, environment‐friendly process based on very low‐dose ultra‐violet irradiation from KrCl (222 nm) Xe 2 (172 excimer demonstrated. The performance commercial BOPP boosted in terms withstanding electric‐field extremes (Weibull breakdown strength 694 to 811 V µm −1 by 17% at 25 °C 428 651 52% 120 °C), discharged energy density, conduction losses. Importantly, depth profile space charge precisely measured situ with high resolution 500 nm laser induced pressure pulse. Consequently, effect distortion are reduced related improved polymer films. It demonstrated that energetic UV photons act as scissors chains dissociate oxygen molecules leading more thermally stable oxygen‐containing structures, deep traps impede migration. This work provides promising approach produce polymers customized microscopic characteristics compatible assembly lines polymer‐based capacitors.

Language: Английский

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Boosting the Strength and Toughness of Polymer Blends via Ligand‐Modulated MOFs

Advanced Science, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 16, 2024

Abstract Mechanically robust and tough polymeric materials are in high demand for applications ranging from flexible electronics to aerospace. However, achieving both toughness strength polymers remains a significant challenge due their inherently contradictory nature. Here, universal strategy enhancing the of polymer blends using ligand‐modulated metal–organic framework (MOF) nanoparticles is presented, which engineered have adjustable hydrophilicity lipophilicity by varying types ratios ligands. Molecular dynamics (MD) simulations demonstrate that these can effectively regulate interfaces between chemically distinct based on amphiphilicity. Remarkably, mere 0.1 wt.% MOF with optimized amphiphilicity (ML‐MOF (5:5) ) delivered ≈1.1‐ ≈34.1‐fold increase poly (lactic acid) (PLA)/poly (butylene succinate) (PBS) blend, respectively. Moreover, amphiphilicity‐tailorable universally enhance mechanical properties various blends, such as polypropylene (PP)/polyethylene (PE), PP/polystyrene (PS), PLA/poly adipate‐co‐terephthalate) (PBAT), PLA/polycaprolactone (PCL)/PBS. This simple method offers potential strengthening toughening blends.

Language: Английский

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Lifecycle Management for Sustainable Plastics: Recent Progress from Synthesis, Processing to Upcycling

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(33)

Published: June 13, 2024

Abstract Plastics, renowned for their outstanding properties and extensive applications, assume an indispensable irreplaceable role in modern society. However, the ubiquitous consumption of plastic items has led to a growing accumulation waste. Unreasonable practices production, utilization, recycling plastics have substantial energy resource depletion environmental pollution. Herein, state‐of‐the‐art advancements lifecycle management are timely reviewed. Unlike typical reviews focused on recycling, this work presents in‐depth analysis entire plastics, covering whole process from synthesis, processing, ultimate disposal. The primary emphasis lies selecting judicious strategies methodologies at each stage mitigate adverse impact waste plastics. Specifically, article delineates rationale, methods, realized various stages through both physical chemical pathways. focal point is attainment optimal rates thereby alleviating ecological burden By scrutinizing aims furnish comprehensive solutions reducing pollution fostering sustainability across all facets

Language: Английский

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Upcycling Polyolefin Blends into High-Performance Materials by Exploiting Azidotriazine Chemistry Using Reactive Extrusion

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(4), P. 2673 - 2684

Published: Jan. 18, 2024

The revalorization of incompatible polymer blends is a key obstacle in realizing circular economy the plastics industry. Polyolefin waste particularly challenging because it difficult to sort into its constituent components. Untreated polyethylene and polypropylene typically exhibit poor mechanical properties that are suitable only for low-value applications. Herein, we disclose simple azidotriazine-based grafting agent enables polyolefin be directly upcycled high-performance materials by using reactive extrusion at industrially relevant processing temperatures. Based on series model experiments, azidotriazine thermally decomposes form triplet nitrene species, which subsequently undergoes complex mixture grafting, oligomerization, cross-linking reactions; strikingly, oligomerization reactions proceed through formation nitrogen-nitrogen bonds. When applied during extrusion, this combination leads generation amorphous, phase-separated nanostructures tend exist polymer-polymer interfaces. These act as multivalent cross-linkers reinforce resulting material, leading dramatically improved ductility compared with untreated blends, along high dimensional stability temperatures excellent recyclability. We propose unique behavior derived from thermomechanically activated reversibility bonds make up structures. Finally, scope chemistry demonstrated applying ternary well postconsumer feedstocks.

Language: Английский

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Structure–Property Relationships of Elastomeric Vinylogous Urethane Thermosets and Their Application as Closed-Loop Recyclable Strain Sensors

Macromolecules, Journal Year: 2025, Volume and Issue: 58(4), P. 1923 - 1934

Published: Feb. 5, 2025

Developing closed-loop recyclable thermosets and understanding their structure–property relationships are essential steps in advancing a circular materials economy. Here, we present vinylogous urethane (VU) thermoset with recyclability, synthesized through the reaction of polytetrahydrofuran bisacetoacetate (aPTHF) tris(2-aminoethyl)amine (TREN). These VU polymers exhibit high elasticity, only 3–9% residual strain observed after cyclic tensile testing at maximum 100%, depending on molecular weight aPTHF network cross-link density. The two structural parameters also allow modulation mechanical stress-relaxation properties elastomers. To investigate hydrolysis linkages within hydrophobic matrix, employed heterogeneous system using biphasic mixture HCl CDCl3. Our findings show that VUs remain stable pure water but can be dissociated under acidic conditions, dissociation rate accelerated higher temperatures and/or presence concentrations. detailed investigations indicate potential elastomers as sustainable substrates for wearable sensors. We therefore conduct case study synthesizing sensor incorporation multiwalled carbon nanotubes (MCNs) into elastomer matrix. robustly detect various movements. Moreover, treatment both neat polymer composite diethyl ether solvent allows excellent recovery (>90%) TREN (86%), without discernible damage to MCNs reclaimed from latter.

Language: Английский

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Circular Polyolefins: Advances toward a Sustainable Future

Macromolecules, Journal Year: 2023, Volume and Issue: 56(15), P. 5679 - 5697

Published: July 21, 2023

Plastics offer several advantages, but their production and disposal processes have severe environmental implications. To overcome these issues, there is a need to switch from the linear circular economy by recycling plastic waste utilizing renewable resources create bioplastics. However, this challenging in case of nonbiodegradable polyolefins (POs), which form largest fraction produced polymers least recycled one. Mechanical recycling, chemical PO bioplastics are three pillars economy. Although mechanical an environmentally economically viable option, it often results degradation downgrading POs. Nonetheless, innovations such as use (nano)fillers or compatibilization with olefin block copolymers, attempt mitigate issues. Furthermore, development covalent adaptable networks improves properties thermoplastics provides recyclable elastomers. If fails meet desired characteristics recyclate PO, other chemicals potential alternative. retrieving monomer ideal for achieving closed-loop economy, traditional approaches noncatalytic POs energy-intensive lack specificity. This has been tried be addressed advancements catalytic approaches. Finally, biobased polyolefins, especially those through emerging nonbiochemical approaches, attractive alternatives that can integrated into existing petrochemical plants. With comprehensive perspective on academic industrial researchers field better contribute more sustainable future.

Language: Английский

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MatGPT: A Vane of Materials Informatics from Past, Present, to Future

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(6)

Published: Oct. 10, 2023

Abstract Combining materials science, artificial intelligence (AI), physical chemistry, and other disciplines, informatics is continuously accelerating the vigorous development of new materials. The emergence “GPT (Generative Pre‐trained Transformer) AI” shows that scientific research field has entered era intelligent civilization with “data” as basic factor “algorithm + computing power” core productivity. continuous innovation AI will impact cognitive laws methods, reconstruct knowledge wisdom system. This leads to think more about informatics. Here, a comprehensive discussion models infrastructures provided, advances in discovery design are reviewed. With rise paradigms triggered by “AI for Science”, vane informatics: “MatGPT”, proposed technical path planning from aspects data, descriptors, generative models, pretraining directed collaborative training, experimental robots, well efforts preparations needed develop generation informatics, carried out. Finally, challenges constraints faced discussed, order achieve digital, intelligent, automated construction joint interdisciplinary scientists.

Language: Английский

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