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      Electrocatalytic upcycling of polyethylene terephthalate to commodity chemicals and H 2 fuel

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          Abstract

          Plastic wastes represent a largely untapped resource for manufacturing chemicals and fuels, particularly considering their environmental and biological threats. Here we report electrocatalytic upcycling of polyethylene terephthalate (PET) plastic to valuable commodity chemicals (potassium diformate and terephthalic acid) and H 2 fuel. Preliminary techno-economic analysis suggests the profitability of this process when the ethylene glycol (EG) component of PET is selectively electrooxidized to formate (>80% selectivity) at high current density (>100 mA cm −2). A nickel-modified cobalt phosphide (CoNi 0.25P) electrocatalyst is developed to achieve a current density of 500 mA cm −2 at 1.8 V in a membrane-electrode assembly reactor with >80% of Faradaic efficiency and selectivity to formate. Detailed characterizations reveal the in-situ evolution of CoNi 0.25P catalyst into a low-crystalline metal oxy(hydroxide) as an active state during EG oxidation, which might be responsible for its advantageous performances. This work demonstrates a sustainable way to implement waste PET upcycling to value-added products.

          Abstract

          Plastic upcycling to value-added products is of great interests. Here the authors investigate a nickel-cobalt phosphide electrocatalyst for electroreforming of polyethylene terephthalate plastic toward valuable potassium diformate, terephthalic acid, and H 2 fuel.

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          Most cited references53

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          Production, use, and fate of all plastics ever made

          We present the first ever global account of the production, use, and end-of-life fate of all plastics ever made by humankind.
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            What would it take for renewably powered electrosynthesis to displace petrochemical processes?

            Electrocatalytic transformation of carbon dioxide (CO 2 ) and water into chemical feedstocks offers the potential to reduce carbon emissions by shifting the chemical industry away from fossil fuel dependence. We provide a technoeconomic and carbon emission analysis of possible products, offering targets that would need to be met for economically compelling industrial implementation to be achieved. We also provide a comparison of the projected costs and CO 2 emissions across electrocatalytic, biocatalytic, and fossil fuel–derived production of chemical feedstocks. We find that for electrosynthesis to become competitive with fossil fuel–derived feedstocks, electrical-to-chemical conversion efficiencies need to reach at least 60%, and renewable electricity prices need to fall below 4 cents per kilowatt-hour. We discuss the possibility of combining electro- and biocatalytic processes, using sequential upgrading of CO 2 as a representative case. We describe the technical challenges and economic barriers to marketable electrosynthesized chemicals.
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              An engineered PET depolymerase to break down and recycle plastic bottles

              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.
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                Author and article information

                Contributors
                hhduan@mail.tsinghua.edu.cn
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                17 August 2021
                17 August 2021
                2021
                : 12
                : 4679
                Affiliations
                [1 ]GRID grid.12527.33, ISNI 0000 0001 0662 3178, Department of Chemistry, , Tsinghua University, ; Beijing, China
                [2 ]GRID grid.48166.3d, ISNI 0000 0000 9931 8406, State Key Laboratory of Chemical Resource Engineering, College of Chemistry, , Beijing University of Chemical Technology, ; Beijing, China
                [3 ]GRID grid.9227.e, ISNI 0000000119573309, Institute of High Energy Physics, , The Chinese Academy of Sciences, ; Beijing, China
                Author information
                http://orcid.org/0000-0002-7521-5837
                http://orcid.org/0000-0003-3210-0068
                Article
                25048
                10.1038/s41467-021-25048-x
                8371182
                34404779
                9f2be16d-8d67-4808-9f3f-d8b691237bd0
                © The Author(s) 2021

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 10 April 2021
                : 9 July 2021
                Funding
                Funded by: FundRef https://doi.org/10.13039/501100001809, National Natural Science Foundation of China (National Science Foundation of China);
                Award ID: 21978147
                Award ID: 21935001
                Award Recipient :
                Funded by: FundRef https://doi.org/10.13039/501100004826, Natural Science Foundation of Beijing Municipality (Beijing Natural Science Foundation);
                Award ID: 2214063
                Award Recipient :
                Categories
                Article
                Custom metadata
                © The Author(s) 2021

                Uncategorized
                sustainability,electrocatalysis,renewable energy,nanoparticles
                Uncategorized
                sustainability, electrocatalysis, renewable energy, nanoparticles

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