Computational Redesign of a PETase for Plastic Biodegradation under Ambient Condition by the GRAPE Strategy

ACS Catalysis, Год журнала: 2021, Номер 11(3), С. 1340 - 1350

Опубликована: Янв. 13, 2021

Nature has provided a fantastic array of enzymes that are responsible for essential biochemical functions but not usually suitable technological applications. Not content with the natural repertoire, protein engineering holds promise to extend applications improved tailored properties. However, robust proteins remains difficult task since positive mutation library may cooperate reach target function in most cases owing ubiquity epistatic effects. The main demand lies identifying an efficient path accumulated mutations. Herein, we devised computational strategy (greedy engineering, GRAPE) improve robustness PETase from Ideonella sakaiensis. A systematic clustering analysis combined greedy accumulation beneficial mutations computationally derived enabled redesign variant, DuraPETase, which exhibits apparent melting temperature is drastically elevated by 31 °C and strikingly enhanced degradation toward semicrystalline poly(ethylene terephthalate) (PET) films (30%) at mild temperatures (over 300-fold). Complete biodegradation 2 g/L microplastics water-soluble products under conditions also achieved, opening up opportunities steer biological uncollectable PET waste further conversion resulting monomers high-value molecules. crystal structure revealed individual match design model. Concurrently, synergistic effects captured, while interactions alleviated during process. We anticipate our will provide broadly applicable global optimization enzyme performance.

Язык: Английский

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Polyethylene terephthalate (PET) in the packaging industry

Polymer Testing, Год журнала: 2020, Номер 90, С. 106707 - 106707

Опубликована: Июль 28, 2020

Язык: Английский

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Catalytic processing of plastic waste on the rise

Chem, Год журнала: 2021, Номер 7(6), С. 1487 - 1533

Опубликована: Янв. 10, 2021

Язык: Английский

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Characterization and engineering of a two-enzyme system for plastics depolymerization

Proceedings of the National Academy of Sciences, Год журнала: 2020, Номер 117(41), С. 25476 - 25485

Опубликована: Сен. 28, 2020

Significance Deconstruction of recalcitrant polymers, such as cellulose or chitin, is accomplished in nature by synergistic enzyme cocktails that evolved over millions years. In these systems, soluble dimeric oligomeric intermediates are typically released via interfacial biocatalysis, and additional enzymes often process the into monomers for microbial uptake. The recent discovery a two-enzyme system polyethylene terephthalate (PET) deconstruction, which employs one to convert polymer another produce constituent PET (MHETase), suggests may be evolving similar deconstruction strategies synthetic plastics. This study on characterization MHETase synergy depolymerization inform cocktail-based plastics upcycling.

Язык: Английский

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Structure of the plastic-degrading Ideonella sakaiensis MHETase bound to a substrate

Nature Communications, Год журнала: 2019, Номер 10(1)

Опубликована: Апрель 12, 2019

Abstract The extreme durability of polyethylene terephthalate (PET) debris has rendered it a long-term environmental burden. At the same time, current recycling efforts still lack sustainability. Two recently discovered bacterial enzymes that specifically degrade PET represent promising solution. First, Ideonella sakaiensis PETase, structurally well-characterized consensus α/β-hydrolase fold enzyme, converts to mono-(2-hydroxyethyl) (MHET). MHETase, second key hydrolyzes MHET educts and ethylene glycol. Here, we report crystal structures active ligand-free MHETase bound nonhydrolyzable analog. which is reminiscent feruloyl esterases, possesses classic domain lid conferring substrate specificity. In light structure-based mapping site, activity assays, mutagenesis studies first structure-guided alteration specificity towards bis-(2-hydroxyethyl) (BHET) reported here, anticipate be valuable resource further advance enzymatic plastic degradation.

Язык: Английский

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Catalytic upcycling of high-density polyethylene via a processive mechanism

Nature Catalysis, Год журнала: 2020, Номер 3(11), С. 893 - 901

Опубликована: Окт. 12, 2020

Язык: Английский

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Expanding plastics recycling technologies: chemical aspects, technology status and challenges

Green Chemistry, Год журнала: 2022, Номер 24(23), С. 8899 - 9002

Опубликована: Янв. 1, 2022

This paper reviewed the entire life cycle of plastics and options for management plastic waste to address barriers industrial chemical recycling further provide perceptions on possible opportunities with such materials.

Язык: Английский

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Enzymatic degradation of plant biomass and synthetic polymers

Nature Reviews Chemistry, Год журнала: 2020, Номер 4(3), С. 114 - 126

Опубликована: Фев. 21, 2020

Язык: Английский

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Enzymes’ Power for Plastics Degradation

Chemical Reviews, Год журнала: 2023, Номер 123(9), С. 5612 - 5701

Опубликована: Март 14, 2023

Plastics are everywhere in our modern way of living, and their production keeps increasing every year, causing major environmental concerns. Nowadays, the end-of-life management involves accumulation landfills, incineration, recycling to a lower extent. This ecological threat environment is inspiring alternative bio-based solutions for plastic waste treatment toward circular economy. Over past decade, considerable efforts have been made degrade commodity plastics using biocatalytic approaches. Here, we provide comprehensive review on recent advances enzyme-based biocatalysis design related processes recycle or upcycle plastics, including polyesters, polyamides, polyurethanes, polyolefins. We also discuss scope limitations, challenges, opportunities this field research. An important message from that polymer-assimilating enzymes very likely part solution reaching

Язык: Английский

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Techno-economic, life-cycle, and socioeconomic impact analysis of enzymatic recycling of poly(ethylene terephthalate)

Joule, Год журнала: 2021, Номер 5(9), С. 2479 - 2503

Опубликована: Июль 15, 2021

Esterases have emerged as important biocatalysts for enzyme-based polyester recycling of poly(ethylene terephthalate) (PET) to terephthalic acid (TPA) and ethylene glycol (EG). Here, we present process modeling, techno-economic, life-cycle, socioeconomic impact analyses an enzymatic PET depolymerization-based process, which compare with virgin TPA manufacturing. We predict that enzymatically recycled (rTPA) can be cost-competitive highlight key areas achieve this. In addition favorable long-term benefits, rTPA reduce total supply chain energy use by 69%–83% greenhouse gas emissions 17%–43% per kg TPA. An economy-wide assessment the US estimates environmental impacts up 95% while generating 45% more also relative production. Sensitivity impactful research opportunities pursue toward realizing biological upcycling.

Язык: Английский

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