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1.
Nature ; 631(8022): 884-890, 2024 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-39020178

RESUMEN

Plastic production reached 400 million tons in 2022 (ref. 1), with packaging and single-use plastics accounting for a substantial amount of this2. The resulting waste ends up in landfills, incineration or the environment, contributing to environmental pollution3. Shifting to biodegradable and compostable plastics is increasingly being considered as an efficient waste-management alternative4. Although polylactide (PLA) is the most widely used biosourced polymer5, its biodegradation rate under home-compost and soil conditions remains low6-8. Here we present a PLA-based plastic in which an optimized enzyme is embedded to ensure rapid biodegradation and compostability at room temperature, using a scalable industrial process. First, an 80-fold activity enhancement was achieved through structure-based rational engineering of a new hyperthermostable PLA hydrolase. Second, the enzyme was uniformly dispersed within the PLA matrix by means of a masterbatch-based melt extrusion process. The liquid enzyme formulation was incorporated in polycaprolactone, a low-melting-temperature polymer, through melt extrusion at 70 °C, forming an 'enzymated' polycaprolactone masterbatch. Masterbatch pellets were integrated into PLA by melt extrusion at 160 °C, producing an enzymated PLA film (0.02% w/w enzyme) that fully disintegrated under home-compost conditions within 20-24 weeks, meeting home-composting standards. The mechanical and degradation properties of the enzymated film were compatible with industrial packaging applications, and they remained intact during long-term storage. This innovative material not only opens new avenues for composters and biomethane production but also provides a feasible industrial solution for PLA degradation.


Asunto(s)
Plásticos Biodegradables , Biodegradación Ambiental , Enzimas Inmovilizadas , Hidrolasas , Poliésteres , Ingeniería de Proteínas , Plásticos Biodegradables/química , Plásticos Biodegradables/metabolismo , Enzimas Inmovilizadas/química , Enzimas Inmovilizadas/metabolismo , Hidrolasas/metabolismo , Hidrolasas/química , Poliésteres/química , Poliésteres/metabolismo , Suelo/química , Temperatura , Estabilidad de Enzimas , Compostaje
2.
Nature ; 580(7802): 216-219, 2020 04.
Artículo en Inglés | MEDLINE | ID: mdl-32269349

RESUMEN

Present estimates suggest that of the 359 million tons of plastics produced annually worldwide1, 150-200 million tons accumulate in landfill or in the natural environment2. Poly(ethylene terephthalate) (PET) is the most abundant polyester plastic, with almost 70 million tons manufactured annually worldwide for use in textiles and packaging3. The main recycling process for PET, via thermomechanical means, results in a loss of mechanical properties4. Consequently, de novo synthesis is preferred and PET waste continues to accumulate. With a high ratio of aromatic terephthalate units-which reduce chain mobility-PET is a polyester that is extremely difficult to hydrolyse5. Several PET hydrolase enzymes have been reported, but show limited productivity6,7. Here we describe an improved PET hydrolase that ultimately achieves, over 10 hours, a minimum of 90 per cent PET depolymerization into monomers, with a productivity of 16.7 grams of terephthalate per litre per hour (200 grams per kilogram of PET suspension, with an enzyme concentration of 3 milligrams per gram of PET). This highly efficient, optimized enzyme outperforms all PET hydrolases reported so far, including an enzyme8,9 from the bacterium Ideonella sakaiensis strain 201-F6 (even assisted by a secondary enzyme10) and related improved variants11-14 that have attracted recent interest. We also show that biologically recycled PET exhibiting the same properties as petrochemical PET can be produced from enzymatically depolymerized PET waste, before being processed into bottles, thereby contributing towards the concept of a circular PET economy.


Asunto(s)
Hidrolasas/química , Hidrolasas/metabolismo , Plásticos/química , Plásticos/metabolismo , Tereftalatos Polietilenos/química , Tereftalatos Polietilenos/metabolismo , Ingeniería de Proteínas , Reciclaje , Actinobacteria/enzimología , Burkholderiales/enzimología , Hidrolasas de Éster Carboxílico/química , Hidrolasas de Éster Carboxílico/metabolismo , Disulfuros/química , Disulfuros/metabolismo , Pruebas de Enzimas , Estabilidad de Enzimas , Fusarium/enzimología , Modelos Moleculares , Ácidos Ftálicos/metabolismo , Polimerizacion , Thermobifida
3.
Aquat Toxicol ; 65(2): 117-40, 2003 Oct 29.
Artículo en Inglés | MEDLINE | ID: mdl-12946614

RESUMEN

Bioaccumulation of Cd, Pb, Cu and Zn in the Antarctic gammaridean amphipod Paramoera walkeri (Stebbing, 1906) was investigated at Casey station (Australian Antarctic Territory). The main goals were to provide information on accumulation strategies of the organisms tested and to verify toxicokinetic models as a predictive tool. The organisms accumulated metals upon exposure and it was possible to estimate significant model parameters of two-compartment and hyperbolic models. These models were successfully verified in a second toxicokinetic study. However, the application of hyperbolic models appears to be more promising as a predictive tool for metals in amphipods compared to compartment models, which have failed to adequately predict metal accumulation in experiments with increasing external exposures in previous studies. The following kinetic bioconcentration factors (BCFs) for the theoretical equilibrium were determined: 150-630 (Cd), 1600-7000 (Pb), 1700-3800 (Cu) and 670-2400 (Zn). We find decreasing BCFs with increasing external metal dosing but similar results for treatments with and without natural UV radiation and for the combined effect of different exposure regimes (single versus multiple metal exposure) and/or the amphipod collective involved (Beall versus Denison Island). A tentative estimation showed the following sequence of sensitivity of P. walkeri to an increase of soluble metal exposure: 0.2-3.0 microg Cd l(-1), 0.12-0.25 microg Pb l(-1), 0.9-3.0 microg Cu l(-1) and 9-26 microg Zn l(-1). Thus, the amphipod investigated proved to be more sensitive as biomonitor compared to gammarids from German coastal waters (with the exception of Cd) and to copepods from the Weddell Sea inferred from literature data.


Asunto(s)
Anfípodos/metabolismo , Metales Pesados/farmacocinética , Contaminantes Químicos del Agua/farmacocinética , Anfípodos/química , Animales , Regiones Antárticas , Carga Corporal (Radioterapia) , Monitoreo del Ambiente/métodos , Metales Pesados/toxicidad , Modelos Biológicos , Océanos y Mares , Luz Solar , Rayos Ultravioleta , Contaminantes Químicos del Agua/toxicidad
4.
Environ Toxicol Chem ; 20(9): 2088-92, 2001 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-11521839

RESUMEN

Investigations on the combined effects of ultraviolet (UV)-B radiation and anthropogenic toxicants have focused primarily on the chemical interactions between UV-B and organic compounds. Only a few studies have examined whether exposure to UV-B changes sensitivity to toxicants. This question is addressed in a laboratory study using the common shoreline Antarctic amphipod Paramoera walkeri and exposure to environmentally realistic levels of copper, UV-B radiation, and food shortage. Exposure to copper for 21 d in the absence of any additional stressors (food present, no UV-B) showed a lowest observable effective concentration (LOEC) of greater than 100 microg Cu/L. Exposure to copper and UV-B in combination, with no shortage of food, resulted in a LOEC of 45 microg Cu/L. When exposed to copper and UV-B, with shortage of food, a LOEC of 3 microg Cu/L was recorded. Hence, the combination of environmental stress from exposure to UV-B radiation and shortage of food increases the sensitivity of P. walkeri to copper more than 30-fold. Increased metabolic energy requirements for defense mechanisms in response to toxicants and UV-B are discussed as possible explanations. It is concluded that consideration of environmental stressors in combination with toxicants increases the accuracy of ecological risk assessments of toxicants and should be part of the process for developing guidelines for ecologically acceptable concentrations of contaminants in the environment.


Asunto(s)
Cobre/efectos adversos , Crustáceos , Privación de Alimentos , Rayos Ultravioleta/efectos adversos , Contaminantes del Agua/efectos adversos , Adaptación Fisiológica , Animales , Dosificación Letal Mediana , Medición de Riesgo
5.
Aquat Toxicol ; 49(1-2): 131-143, 2000 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-10814812

RESUMEN

This study provides information on LC(50) toxicity tests and bioaccumulation of heavy metals in the nearshore Antarctic gammarid, Paramorea walkeri. The 4 day LC(50) values were 970 µg/l for copper and 670 µg/l for cadmium. Net uptake rates and bioconcentration factors of these elements were determined under laboratory conditions. After 12 days of exposure to 30 µg/l, the net uptake rates were 5.2 and 0.78 µg/g per day and the bioconcentration factors were 2080 and 311 for copper and cadmium, respectively. The body concentrations of copper were significantly correlated with the concentrations of this element in the water. Accumulation of copper and cadmium continued for the entire exposure suggesting that heavy metals concentrations were not regulated to constant concentrations in the body. Using literature data about two compartments (water-animal) first-order kinetic models, a very good agreement was found between body concentrations observed after exposure and model predicted. Exposure of P. walkeri to mixtures of copper and cadmium showed that accumulation of these elements can be assessed by addition of results obtained from single exposure, with only a small degree of uncertainty. The study provides information on the sensitivity of one Antarctic species towards contaminants, and the results were compared with data of similar species from lower latitudes. An important finding is that sensitivity to toxic chemicals and toxicokinetic parameters in the species investigated are comparable with those of non-polar species. The characteristics of bioaccumulation demonstrate that P. walkeri is a circumpolar species with the potential to be a standard biological indicator for use in monitoring programmes of Antarctic nearshore ecosystems. The use of model prediction provide further support to utilise these organisms for biomonitoring.

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