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1.
J Environ Sci (China) ; 147: 523-537, 2025 Jan.
Article in English | MEDLINE | ID: mdl-39003068

ABSTRACT

Due to its high efficiency, Fe(II)-based catalytic oxidation has been one of the most popular types of technology for treating growing organic pollutants. A lot of chemical Fe sludge along with various refractory pollutants was concomitantly produced, which may cause secondary environmental problems without proper disposal. We here innovatively proposed an effective method of achieving zero Fe sludge, reusing Fe resources (Fe recovery = 100%) and advancing organics removal (final TOC removal > 70%) simultaneously, based on the in situ formation of magnetic Ca-Fe layered double hydroxide (Fe3O4@CaFe-LDH) nano-material. Cations (Ca2+ and Fe3+) concentration (≥ 30 mmol/L) and their molar ratio (Ca:Fe ≥ 1.75) were crucial to the success of the method. Extrinsic nano Fe3O4 was designed to be involved in the Fe(II)-catalytic wastewater treatment process, and was modified by oxidation intermediates/products (especially those with COO- structure), which promoted the co-precipitation of Ca2+ (originated from Ca(OH)2 added after oxidation process) and by-produced Fe3+ cations on its surface to in situ generate core-shell Fe3O4@CaFe-LDH. The oxidation products were further removed during Fe3O4@CaFe-LDH material formation via intercalation and adsorption. This method was applicable to many kinds of organic wastewater, such as bisphenol A, methyl orange, humics, and biogas slurry. The prepared magnetic and hierarchical CaFe-LDH nanocomposite material showed comparable application performance to the recently reported CaFe-LDHs. This work provides a new strategy for efficiently enhancing the efficiency and economy of Fe(II)-catalyzed oxidative wastewater treatment by producing high value-added LDHs materials.


Subject(s)
Oxidation-Reduction , Waste Disposal, Fluid , Wastewater , Water Pollutants, Chemical , Water Pollutants, Chemical/chemistry , Waste Disposal, Fluid/methods , Wastewater/chemistry , Catalysis , Iron/chemistry
2.
J Environ Sci (China) ; 147: 93-100, 2025 Jan.
Article in English | MEDLINE | ID: mdl-39003087

ABSTRACT

Polybromodiphenyl ethers (PBDEs), the widely used flame retardants, are common contaminants in surface soils at e-waste recycling sites. The association of PBDEs with soil colloids has been observed, indicating the potential risk to groundwater due to colloid-facilitated transport. However, the extent to which soil colloids may enhance the spreading of PBDEs in groundwater is largely unknown. Herein, we report the co-transport of decabromodiphenyl ester (BDE-209) and soil colloids in saturated porous media. The colloids released from a soil sample collected at an e-waste recycling site in Tianjin, China, contain high concentration of PBDEs, with BDE-209 being the most abundant conger (320 ± 30 mg/kg). The colloids exhibit relatively high mobility in saturated sand columns, under conditions commonly observed in groundwater environments. Notably, under all the tested conditions (i.e., varying flow velocity, pH, ionic species and ionic strength), the mass of eluted BDE-209 correlates linearly with that of eluted soil colloids, even though the mobility of the colloids varies markedly depending on the specific hydrodynamic and solution chemistry conditions involved. Additionally, the mass of BDE-209 retained in the columns also correlates strongly with the mass of retained colloids. Apparently, the PBDEs remain bound to soil colloids during transport in porous media. Findings in this study indicate that soil colloids may significantly promote the transport of PBDEs in groundwater by serving as an effective carrier. This might be the reason why the highly insoluble and adsorptive PBDEs are found in groundwater at some PBDE-contaminated sites.


Subject(s)
Colloids , Flame Retardants , Groundwater , Halogenated Diphenyl Ethers , Soil Pollutants , Soil , Water Pollutants, Chemical , Halogenated Diphenyl Ethers/analysis , Colloids/chemistry , Groundwater/chemistry , Soil Pollutants/analysis , Soil Pollutants/chemistry , Soil/chemistry , Water Pollutants, Chemical/analysis , China , Flame Retardants/analysis , Environmental Monitoring , Models, Chemical
3.
J Environ Sci (China) ; 149: 234-241, 2025 Mar.
Article in English | MEDLINE | ID: mdl-39181638

ABSTRACT

Reducing the cost of RuO2/TiO2 catalysts is still one of the urgent challenges in catalytic HCl oxidation. In the present work, a Ce-doped TiO2 supported RuO2 catalyst with a low Ru loading was developed, showing a high activity in the catalytic oxidation of HCl to Cl2. The results on some extensive characterizations of both Ce-doped TiO2 carriers and their supported RuO2 catalysts show that the doping of Ce into TiO2 can effectively change the lattice parameters of TiO2 to improve the dispersion of the active RuO2 species on the carrier, which facilitates the production of surface Ru species to expose more active sites for boosting the catalytic performance even under some harsh reaction conditions. This work provides some scientific basis and technical support for chlorine recycling.


Subject(s)
Cerium , Hydrochloric Acid , Oxidation-Reduction , Titanium , Titanium/chemistry , Catalysis , Cerium/chemistry , Hydrochloric Acid/chemistry , Ruthenium Compounds/chemistry , Chlorides/chemistry , Models, Chemical , Chlorine/chemistry
4.
Beilstein J Org Chem ; 20: 2129-2142, 2024.
Article in English | MEDLINE | ID: mdl-39224231

ABSTRACT

Organocatalysis has become a powerful tool in synthetic chemistry, providing a cost-effective alternative to traditional catalytic methods. The immobilisation of organocatalysts offers the potential to increase catalyst reusability and efficiency in organic reactions. This article reviews the key parameters that influence the effectiveness of immobilised organocatalysts, including the type of support, immobilisation techniques and the resulting interactions. In addition, the influence of these factors on catalytic activity, selectivity and recyclability is discussed, providing an insight into optimising the performance of immobilised organocatalysts for practical applications in organic chemistry.

5.
Heliyon ; 10(16): e35898, 2024 Aug 30.
Article in English | MEDLINE | ID: mdl-39224352

ABSTRACT

The main objective described in this paper is the optimization of technological parameters in the production of varistors based on recycled zinc oxide (ZnO). The content of this paper builds on our previous research aimed at proving that hydrometallurgically recovered ZnO material, from electric arc furnace dust, is suitable for applications in these semiconductors, an issue which has received very little attention at present. The focus of this research also corresponds to and supports the visions and strategies of environmental sustainability and the circular economy. Samples of ZnO varistors manufactured for this purpose were analyzed by scanning electron microscopy and then the electrical parameters were measured and calculated. Based on the results of the microstructural analysis and electrical properties, prerequisites for the optimal adjustment of technological parameters such as sintering temperature and sintering time were derived, which will be the starting point for further research.

6.
Compr Rev Food Sci Food Saf ; 23(5): e70011, 2024 Sep.
Article in English | MEDLINE | ID: mdl-39223762

ABSTRACT

Food waste is a serious worldwide issue that has an impact on the environment, society, and economy. This comprehensive review provides a detailed description of methods and approaches for reducing food waste, emphasizing the necessity of comprehensive strategies to tackle its intricate relationship with environmental sustainability, social equity, and economic prosperity. By scrutinizing the extent and impact of food waste, from initial production stages to final disposal, this comprehensive review underlines the urgent need for integrated solutions that include technological advancements, behavioral interventions, regulatory frameworks, and collaborative endeavors. Environmental assessments highlight the significant contribution of food waste to greenhouse gas emissions, land degradation, water scarcity, and energy inefficiency, thereby emphasizing the importance of curtailing its environmental impact. Concurrently, the social and economic consequences of food waste, such as food insecurity, economic losses, and disparities in food access, underscore the imperative for coordinated action across multiple sectors. Food waste can also be effectively reduced by various innovative approaches, such as technological waste reduction solutions, supply chain optimization strategies, consumer behavior-focused initiatives, and waste recovery and recycling techniques. Furthermore, in order to foster an environment that encourages the reduction of food waste and facilitates the transition to a circular economy, legislative changes and regulatory actions are essential. By embracing these multifaceted strategies and approaches, stakeholders can unite to confront the global food waste crisis, thereby fostering resilience, sustainability, and social equity within our food systems.


Subject(s)
Recycling , Waste Management , Recycling/methods , Waste Management/methods , Food Supply , Food , Food Loss and Waste
7.
Adv Mater ; : e2407854, 2024 Sep 03.
Article in English | MEDLINE | ID: mdl-39225419

ABSTRACT

Thermosets are well known for their advantages such as high stability and chemical resistance. However, developing sustainable thermosets with degradability and recyclability faces several principal challenges, including reconciling the desired characteristics during service with the recycling and reprocessing properties required at the end of life, establishing efficient methods for large-scale synthesis, and aligning with current manufacturing process. Here a general strategy is presented for the on-demand degradation and recycling of thermosets under mild conditions utilizing dynamic precursors with dual-factor-controlled reversibility. Specifically, dynamic triazine crosslinkers are introduced through dynamic nucleophilic aromatic substitution (SNAr) into the precursor polyols used in polyurethane (PU) synthesis. Upon removal of the catalyst and alcohol, the reversibility of SNAr is deactivated, allowing for the use of standard PU polymerization techniques such as injection molding, casting, and foaming. The resulting cyanurate-crosslinked PUs maintain high stability and diverse mechanical properties of traditional crosslinked PUs, yet offer the advantage of easy on-demand depolymerization for recycling by activating the reversibility of SNAr under specific but mild conditions-a combination of base, alcohol, and mild heat. It is envisioned that this approach, involving the pre-installation of dual-factor-controlled dynamic crosslinkers, can be broadly applied to current thermosetting plastic manufacturing processes, introducing enhanced sustainability.

8.
Int J Biol Macromol ; : 135231, 2024 Aug 30.
Article in English | MEDLINE | ID: mdl-39218188

ABSTRACT

Endowing biodegradable plastics with easy recyclability can reduce competition with food resources and further enhance their environmental friendliness. In this work, 4-carboxyphenylboronic acid was grafted onto the side chains of hydroxyethyl cellulose and compounded with inexpensive cornstarch. Upon the introduction of tannic acid, stable and reversible borate ester bond rapidly formed, yielding composite biodegradable plastic films with outstanding mechanical properties and facile recyclability. The formation of a dynamic cross-linked network mitigates the aggregation of gelatinized starch molecules, enhancing the flexibility and durability of the crosslinked film. Testing revealed that while maintaining high tensile strength, the elongation at break of the crosslinked film increased by 952.86 %. The static water contact angle was improved from 32.74° to 78.82°, with a change of <5° within 1 min, demonstrating enhanced water resistance. Excellent antioxidant and thermal stability were also characterized, the crosslinked film can be easily dissolved by heating in water at pH = 6.5 and reshaped in water at pH = 7.2. After five times of regeneration, the tensile strength loss was as low as 5.68 %. This eco-friendly and efficient recycling process is promising during green chemistry.

9.
Biotechnol Adv ; : 108438, 2024 Aug 30.
Article in English | MEDLINE | ID: mdl-39218325

ABSTRACT

The transition to renewable energies and electric vehicles has triggered an unprecedented demand for metals. Sustainable development of these technologies relies on effectively managing the lifecycle of critical raw materials, including their responsible sourcing, efficient use, and recycling. Metal recycling from electronic waste (e-waste) is of paramount importance owing to ore exceeding amounts of critical elements and high toxicity of heavy metals and organic pollutants in e-waste to the natural ecosystem and human body. Heterotrophic microbes secrete numerous metal-binding biomolecules such as organic acids, amino acids, cyanide, siderophores, peptides, and biosurfactants which can be utilized for eco-friendly and profitable metal recycling. In this review paper, we presented a critical review of heterotrophic organisms in biomining, and current barriers hampering the industrial application of organic acid bioleaching and biocyanide leaching. We also discussed how these challenges can be surmounted with simple methods (e.g., culture media optimization, separation of microbial growth and metal extraction process) and state-of-the-art biological approaches (e.g., artificial microbial community, synthetic biology, metabolic engineering, advanced fermentation strategies, and biofilm engineering). Lastly, we showcased emerging technologies (e.g., artificially synthesized peptides, siderophores, and biosurfactants) derived from heterotrophs with the potential for inexpensive, low-impact, selective and advanced metal recovery from bioleaching solutions.

10.
Adv Mater ; : e2408463, 2024 Sep 02.
Article in English | MEDLINE | ID: mdl-39221676

ABSTRACT

The burgeoning accumulation of spent lithium-ion batteries (LIBs), a byproduct from the widespread adoption of portable electronics and electric vehicles, necessitates efficient recycling strategies. Direct recycling represents a promising strategy to maximize the value of LIB waste and minimize harmful environmental outcomes. However, current efforts to large-scale direct recycling face challenges stemming from heterophase residues (e.g., Li2CO3, LiOH) in the recycled products and uncontrolled interfacial instability, often requiring repeated washing that generates significant wastewater. Here, a refined direct recycling process is proposed to improve cathode interface stability by leveraging in situ reaction between surface residual lithium species and a weak inorganic acid to form a conformal Li+ conductive coating that stabilizes the regenerated Ni-rich cathodes with significantly reduced water footprint. The findings reveal that the conductive coating also prevents direct contact between contaminants and the cathode surface, thus improving the ambient storage stability. By eliminating the need for extensive washing, this intensified recycling process offers a more sustainable approach with the potential to transition from laboratory to industrial-scale applications, improving both product quality and environmental sustainability.

11.
J Hazard Mater ; 479: 135554, 2024 Aug 17.
Article in English | MEDLINE | ID: mdl-39232354

ABSTRACT

Achieving circularity in the plastic economy predominantly depends on sourcing higher quality recyclates. Packaging plastic poses a significant challenge as it is often not prioritised for collection or recycling initiatives. The presence of additives, such as printing ink, impedes the quality of recyclates. Considering the volume of packaging plastics and the importance of branding (aesthetics and consumer information), ink removal is a critical pre-treatment step. However, the literature is limited, with only 14 studies exploring de-inking processes. Drawing parallels with the detergent laundering process, surfactants have been widely investigated in plastic de-inking, with cationic surfactants proving the most effective with a de-inking efficiency of up to 100%. However, concerns exist regarding the toxic and hazardous nature of the surfactants and chemicals. The average hazard quotient (AHQ) was developed, which compares de-inking chemicals as one of the key findings. AHQ provides a quantitative proxy for the hazards and toxicities, which are qualitatively presented as part of the globally harmonised system (GHS) classification of chemicals. To drive emerging packaging plastic de-inking, including the development of green surfactants (e.g. gamma-valerolactone), this work enables an informed chemical selection minimising potential hazards (rather than creating more adverse effects in plastic recycling processes) and toxicities from plastic waste, fulfilling the objectives of cleaner plastic waste recycling.

12.
Trends Biochem Sci ; 2024 Aug 27.
Article in English | MEDLINE | ID: mdl-39232879

ABSTRACT

The push for industrial sustainability benefits from the use of enzymes as a replacement for traditional chemistry. Biological catalysts, especially those that have been engineered for increased activity, stability, or novel function, and are often greener than alternative chemical approaches. This Review highlights the role of engineered enzymes (and identifies directions for further engineering efforts) in the application areas of greenhouse gas sequestration, fuel production, bioremediation, and degradation of plastic wastes.

13.
Mol Microbiol ; 2024 Sep 05.
Article in English | MEDLINE | ID: mdl-39233599

ABSTRACT

Many bacteria possess proteasomes and a tagging system that is functionally analogous to the ubiquitin system. In this system, Pup, the tagging protein, marks protein targets for proteasomal degradation. Despite the analogy to the ubiquitin system, where the ubiquitin tag is recycled, it remained unclear whether Pup is similarly recycled, given how the bacterial proteasome does not include a depupylase. We previously showed in vitro that as Pup lacks effective proteasome degradation sites, it is released from the proteasome following target degradation, remaining conjugated to a degradation fragment that can be later depupylated. Here, we tested this model in Mycobacterium smegmatis, using a Pup mutant that is effectively degraded by the proteasome. Our findings indicate that Pup recycling not only occurs in vivo but is also essential to maintain normal pupylome levels and to support bacterial survival under starvation conditions. Accordingly, Pup recycling is an essential process in the mycobacterial Pup-proteasome system.

14.
Waste Manag ; 189: 300-313, 2024 Sep 02.
Article in English | MEDLINE | ID: mdl-39226844

ABSTRACT

The plastic industry needs to match the recycling goals set by the EU. Next to technological hurdles, the cost of plastics mechanical recycling is an important modality in this transition. This paper reveals how business economic cost calculation can expose significant pitfalls in the recycling process, by unravelling limitations and boundary conditions, such as scale. By combining the business economic methodology with a Material Flow Analysis, this paper shows the influence of mass retention of products, the capacity of the processing lines, scaling of input capacity, and waste composition on the recycling process and associated costs. Two cases were investigated: (i) the Initial Sorting in a medium size Material Recovery Facility and (ii) an improved mechanical recycling process for flexibles - known as the Quality Recycling Process - consisting of Additional Sorting and Improved Recycling. Assessing the whole recycling chain gives a more holistic insight into the influences of choices and operating parameters on subsequent costs in other parts of the chain and results in a more accurate cost of recycled plastic products. This research concluded that the cost of Initial Sorting of flexibles is 110,08-122,53 EUR/t, while the cost of subsequent Additional Sorting and Improved Recycling ranges from 566,26 EUR/t for rPE Flex to 735,47 EUR/t for rPP Film, these insights can be used to determine a fair price for plastic products. For the Quality Recycling Process it was shown that rationalisation according to the identified pitfalls can reduce the cost per tonne of product by 15-26%.

15.
Article in English | MEDLINE | ID: mdl-39227243

ABSTRACT

The activation of immune cells by pro-inflammatory or immunosuppressive stimuli is followed by the secretion of immunoregulatory cytokines which serve as messengers to activate the immune response in target cells. Although the mechanisms that control the secretion of cytokines by immune cells are not yet fully understood, several key aspects of this process have recently emerged. This review focuses on cytokine release via exocytosis and highlights the routes of cytokine trafficking leading to constitutive and regulated secretion as well as the impact of sorting receptors on this process. We discuss the involvement of cytoskeletal rearrangements in vesicular transport, secretion, and formation of immunological synapses. Finally, we describe the non-classical pathways of cytokine release that are independent of vesicular ER-Golgi transport. Instead, these pathways are based on processing by inflammasome or autophagic mechanisms. Ultimately, understanding the molecular mechanisms behind cytokine release may help to identify potential therapeutic targets in diseases associated with altered immune responses.

16.
Neurotherapeutics ; : e00378, 2024 Sep 02.
Article in English | MEDLINE | ID: mdl-39227284

ABSTRACT

ADAPT-SC (NCT04735432) was designed to evaluate noninferiority of subcutaneous (SC) efgartigimod PH20 to intravenous (IV) efgartigimod in participants with generalized myasthenia gravis (gMG). ADAPT-SC+ (NCT04818671) is an open-label extension study designed to assess long-term safety, tolerability, and efficacy of efgartigimod PH20 SC. Adult participants in ADAPT-SC were randomly assigned to receive a treatment cycle of 4 once-weekly administrations of efgartigimod PH20 SC 1000 â€‹mg or efgartigimod IV 10 â€‹mg/kg, followed by 7 weeks of follow-up. Primary endpoint was percentage change from baseline in total immunoglobulin G (IgG) level at week 4 (1 week after the fourth administration). Secondary efficacy endpoints assessed number and percentage of Myasthenia Gravis Activities of Daily Living (MG-ADL) and Quantitative Myasthenia Gravis (QMG) responders and mean change from baseline in total score for each measure. The primary endpoint was met, demonstrating noninferiority in total IgG reduction between efgartigimod PH20 SC 1000 â€‹mg and efgartigimod IV 10 â€‹mg/kg. Clinically meaningful improvements were seen as early as 1 week following the first administration in both treatment arms, with maximal improvements at week 4. Continued treatment cycles of efgartigimod PH20 SC in ADAPT-SC+ have demonstrated long-term safety and consistent improvements in MG-ADL total score. Findings from ADAPT-SC and ADAPT-SC+ demonstrate similar safety and efficacy as observed in the placebo-controlled ADAPT study. Collectively, these findings support noninferiority between efgartigimod PH20 SC 1000 â€‹mg and efgartigimod IV 10 â€‹mg/kg, as well as long-term safety, tolerability, and efficacy of efgartigimod PH20 SC for treatment of a broad population of patients with gMG.

17.
ChemSusChem ; : e202400698, 2024 Sep 03.
Article in English | MEDLINE | ID: mdl-39227316

ABSTRACT

Poly(ethylene terephthalate) (PET) is a common single-use plastic and a major contributor to plastic waste. PET upcycling through enzymatic depolymerization has drawn significant interests, but lack of robust enzymes in acidic environments remains a challenge. This study investigates in-situ product removal (ISPR) of protons from enzymatic PET depolymerization via a membrane reactor, focusing on the ICCG variant of leaf branch compost cutinase. More than two-fold improvements in overall PET depolymerization and terephthalic acid yields were achieved employing ISPR for an initial PET loading of 10 mgPET mlbuffer-1. The benefit of ISPR was reduced for a lower initial loading of 1 mgPET mlbuffer-1 due to decreased need for pH stabilization of the enzyme-containing solutions. A back-of-envelop analysis suggests that at a modest dilution ratio, ISPR could help achieve savings on caustic base solutions used for pH control in a bioreactor. Our study provides valuable insights for future ISPR developments for enzymatic PET depolymerization, addressing the pressing need for more sustainable solutions towards plastic recycling and environmental conservation.

18.
Cell Commun Signal ; 22(1): 422, 2024 Sep 02.
Article in English | MEDLINE | ID: mdl-39223673

ABSTRACT

Post-translational SUMOylation of nuclear and cytosolic proteins maintains homeostasis in eukaryotic cells and orchestrates programmed responses to changes in metabolic demand or extracellular stimuli. In excitable cells, SUMOylation tunes the biophysical properties and trafficking of ion channels. Ion channel SUMOylation status is determined by the opposing enzyme activities of SUMO ligases and deconjugases. Phosphorylation also plays a permissive role in SUMOylation. SUMO deconjugases have been identified for several ion channels, but their corresponding E3 ligases remain unknown. This study shows PIAS3, a.k.a. KChAP, is a bona fide SUMO E3 ligase for Kv4.2 and HCN2 channels in HEK cells, and endogenous Kv4.2 and Kv4.3 channels in cardiomyocytes. PIAS3-mediated SUMOylation at Kv4.2-K579 increases channel surface expression through a rab11a-dependent recycling mechanism. PKA phosphorylation at Kv4.2-S552 reduces the current mediated by Kv4 channels in HEK293 cells, cardiomyocytes, and neurons. This study shows PKA mediated phosphorylation blocks Kv4.2-K579 SUMOylation in HEK cells and cardiomyocytes. Together, these data identify PIAS3 as a key downstream mediator in signaling cascades that control ion channel surface expression.


Subject(s)
Cyclic AMP-Dependent Protein Kinases , Myocytes, Cardiac , Protein Inhibitors of Activated STAT , Shal Potassium Channels , Sumoylation , Humans , HEK293 Cells , Cyclic AMP-Dependent Protein Kinases/metabolism , Protein Inhibitors of Activated STAT/metabolism , Protein Inhibitors of Activated STAT/genetics , Animals , Myocytes, Cardiac/metabolism , Shal Potassium Channels/metabolism , Shal Potassium Channels/genetics , Phosphorylation , Molecular Chaperones/metabolism , Molecular Chaperones/genetics
19.
J Physiol ; 2024 Aug 14.
Article in English | MEDLINE | ID: mdl-39141823

ABSTRACT

Dynamins are GTPases required for pinching vesicles off the plasma membrane once a critical curvature is reached during endocytosis. Here, we probed dynamin function in central synapses by depleting all three dynamin isoforms in postnatal hippocampal neurons down to negligible levels. We found a decrease in the propensity of evoked neurotransmission as well as a reduction in synaptic vesicle numbers. Recycling of synaptic vesicles during spontaneous or low levels of evoked activity were largely impervious to dynamin depletion, while retrieval of synaptic vesicle components at higher levels of activity was partially arrested. These results suggest the existence of balancing dynamin-independent mechanisms for synaptic vesicle recycling at central synapses. Classical dynamin-dependent mechanisms are not essential for retrieval of synaptic vesicle proteins after quantal single synaptic vesicle fusion, but they become more relevant for membrane retrieval during intense, sustained neuronal activity. KEY POINTS: Loss of dynamin 2 does not impair synaptic transmission. Loss of all three dynamin isoforms mostly affects evoked neurotransmission. Excitatory synapse function is more susceptible to dynamin loss. Spontaneous neurotransmission is only mildly affected by loss of dynamins. Single synaptic vesicle endocytosis is largely dynamin independent.

20.
ChemSusChem ; : e202401595, 2024 Aug 14.
Article in English | MEDLINE | ID: mdl-39141831

ABSTRACT

Polyurethanes (PUs) are highly versatile polymers widely utilized across industries. However, chemical recycling of PU possess significant challenges due to the harsh conditions required, and the formation of complex mixtures of oligomers upon depolymerization. Addressing this inherent lack of recyclability, we developed closed-loop recyclable PU materials by integrating cleavable acetal groups. We present a sustainable and scalable synthesis method for acetal-containing polyols (APs) through aldehyde-diol polycondensation, utilizing reusable heterogeneous catalysis. Three APs with different hydrolytic stabilities depending on the structure of acetal groups were synthesized from formaldehyde, acetaldehyde, and propionaldehyde with 1,6-hexanediol (H16). These APs were employed alongside 4,4'-methylene diisocyanate (MDI) for preparation of PU materials. The resulting PUs exhibited mechanical properties comparable to or surpassing those of conventional PUs, while demonstrating excellent recyclability under acidic conditions. Notably, hydrolysis of PU materials based on acetaldehyde-derived APs yielded remarkable monomer recovery rates, with 89% for H16 and 84% for 4,4'-methylenedianiline, a precursor to MDI. Furthermore, we successfully demonstrated closed-loop recycling by synthesizing APs from recovered H16, resulting in PU materials with identical properties to the original PU. This achievement highlights the potential for establishing a closed-loop recycling system for acetal-containing PUs, contributing to the advancement of a sustainable and circular economy.

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