Tandem chemical deconstruction and biological upcycling of poly(ethylene terephthalate) to β-ketoadipic acid by Pseudomonas putida KT2440

Werner, Allison Z.; Clare, Rita; Mand, Thomas D.; Pardo, Isabel; Ramirez, Kelsey J.; Haugen, Stefan J.; Bratti, Felicia; Dexter, Gara N.; Elmore, Joshua R.; Huenemann, Jay D.; Peabody, V, George L.; Johnson, Christopher W.; Rorrer, Nicholas A.; Salvachúa, Davinia; Guss, Adam M.; Beckham, Gregg T.

doi:10.1016/j.ymben.2021.07.005

Title: Tandem chemical deconstruction and biological upcycling of poly(ethylene terephthalate) to β-ketoadipic acid by Pseudomonas putida KT2440

Abstract

Poly(ethylene terephthalate) (PET) is the most abundantly consumed synthetic polyester and accordingly a major source of plastic waste. The development of chemocatalytic approaches for PET depolymerization to monomers offers new options for open-loop upcycling of PET, which can leverage biological transformations to higher-value products. To that end, here we perform four sequential metabolic engineering efforts in Pseudomonas putida KT2440 to enable the conversion of PET glycolysis products via: (i) ethylene glycol utilization by constitutive expression of native genes, (ii) terephthalate (TPA) catabolism by expression of tphA2_IIA3_IIB_IIA1_II from Comamonas and tpaK from Rhodococcus jostii, (iii) bis(2-hydroxyethyl) terephthalate (BHET) hydrolysis to TPA by expression of PETase and MHETase from Ideonella sakaiensis, and (iv) BHET conversion to a performance-advantaged bioproduct, ß-ketoadipic acid (ßKA) by deletion of pcaIJ. Using this strain, we demonstrate production of 15.1 g/L ßKA from BHET at 76% molar yield in bioreactors and conversion of catalytically depolymerized PET to ßKA. Overall, this work highlights the potential of tandem catalytic deconstruction and biological conversion as a means to upcycle waste PET.

Authors:

;

; Mand, Thomas D.;

; Ramirez, Kelsey J.;

; Bratti, Felicia; Dexter, Gara N.;

; Huenemann, Jay D.; Peabody, V, George L.; Johnson, Christopher W.;

; Salvachúa, Davinia;

;

Publication Date:: Wed Sep 01 00:00:00 EDT 2021

Research Org.:: National Renewable Energy Lab. (NREL), Golden, CO (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Manufacturing Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Bioenergy Technologies Office

OSTI Identifier:: 1807635

Alternate Identifier(s):: OSTI ID: 1814600; OSTI ID: 1818959

Report Number(s):: NREL/JA-2800-80145
Journal ID: ISSN 1096-7176; S1096717621001154; PII: S1096717621001154

Grant/Contract Number:: AC05-00OR22725; AC36-08GO28308

Resource Type:: Published Article

Journal Name:: Metabolic Engineering

Additional Journal Information:: Journal Name: Metabolic Engineering Journal Volume: 67 Journal Issue: C; Journal ID: ISSN 1096-7176

Publisher:: Elsevier

Country of Publication:: Belgium

Language:: English

Subject:: 32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; 54 ENVIRONMENTAL SCIENCES; bio-upcycling; metabolic engineering; MHETase; PETase; plastics upcycling; terephthalic acid

Citation Formats


                    Werner, Allison Z., Clare, Rita, Mand, Thomas D., Pardo, Isabel, Ramirez, Kelsey J., Haugen, Stefan J., Bratti, Felicia, Dexter, Gara N., Elmore, Joshua R., Huenemann, Jay D., Peabody, V, George L., Johnson, Christopher W., Rorrer, Nicholas A., Salvachúa, Davinia, Guss, Adam M., and Beckham, Gregg T. Tandem chemical deconstruction and biological upcycling of poly(ethylene terephthalate) to β-ketoadipic acid by Pseudomonas putida KT2440.  Belgium: N. p., 2021. 
Web.  doi:10.1016/j.ymben.2021.07.005.

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                    Werner, Allison Z., Clare, Rita, Mand, Thomas D., Pardo, Isabel, Ramirez, Kelsey J., Haugen, Stefan J., Bratti, Felicia, Dexter, Gara N., Elmore, Joshua R., Huenemann, Jay D., Peabody, V, George L., Johnson, Christopher W., Rorrer, Nicholas A., Salvachúa, Davinia, Guss, Adam M., & Beckham, Gregg T. Tandem chemical deconstruction and biological upcycling of poly(ethylene terephthalate) to β-ketoadipic acid by Pseudomonas putida KT2440.  Belgium.  https://doi.org/10.1016/j.ymben.2021.07.005

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                    Werner, Allison Z., Clare, Rita, Mand, Thomas D., Pardo, Isabel, Ramirez, Kelsey J., Haugen, Stefan J., Bratti, Felicia, Dexter, Gara N., Elmore, Joshua R., Huenemann, Jay D., Peabody, V, George L., Johnson, Christopher W., Rorrer, Nicholas A., Salvachúa, Davinia, Guss, Adam M., and Beckham, Gregg T. Wed .  
"Tandem chemical deconstruction and biological upcycling of poly(ethylene terephthalate) to β-ketoadipic acid by Pseudomonas putida KT2440".  Belgium.  https://doi.org/10.1016/j.ymben.2021.07.005.

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@article{osti_1807635,

  title        = {Tandem chemical deconstruction and biological upcycling of poly(ethylene terephthalate) to β-ketoadipic acid by Pseudomonas putida KT2440},

  author       = {Werner, Allison Z. and Clare, Rita and Mand, Thomas D. and Pardo, Isabel and Ramirez, Kelsey J. and Haugen, Stefan J. and Bratti, Felicia and Dexter, Gara N. and Elmore, Joshua R. and Huenemann, Jay D. and Peabody, V, George L. and Johnson, Christopher W. and Rorrer, Nicholas A. and Salvachúa, Davinia and Guss, Adam M. and Beckham, Gregg T.},

  abstractNote = {Poly(ethylene terephthalate) (PET) is the most abundantly consumed synthetic polyester and accordingly a major source of plastic waste. The development of chemocatalytic approaches for PET depolymerization to monomers offers new options for open-loop upcycling of PET, which can leverage biological transformations to higher-value products. To that end, here we perform four sequential metabolic engineering efforts in Pseudomonas putida KT2440 to enable the conversion of PET glycolysis products via: (i) ethylene glycol utilization by constitutive expression of native genes, (ii) terephthalate (TPA) catabolism by expression of tphA2IIA3IIBIIA1II from Comamonas and tpaK from Rhodococcus jostii, (iii) bis(2-hydroxyethyl) terephthalate (BHET) hydrolysis to TPA by expression of PETase and MHETase from Ideonella sakaiensis, and (iv) BHET conversion to a performance-advantaged bioproduct, ß-ketoadipic acid (ßKA) by deletion of pcaIJ. Using this strain, we demonstrate production of 15.1 g/L ßKA from BHET at 76% molar yield in bioreactors and conversion of catalytically depolymerized PET to ßKA. Overall, this work highlights the potential of tandem catalytic deconstruction and biological conversion as a means to upcycle waste PET.},

  doi          = {10.1016/j.ymben.2021.07.005},

  journal      = {Metabolic Engineering},

  number       = C,

  volume       = 67,

  place        = {Belgium},

  year         = {Wed Sep 01 00:00:00 EDT 2021},

  month        = {Wed Sep 01 00:00:00 EDT 2021}

}

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Works referenced in this record:

Aromatic catabolic pathway selection for optimal production of pyruvate and lactate from lignin
journal, March 2015

Johnson, Christopher W.; Beckham, Gregg T.
Metabolic Engineering, Vol. 28
DOI: 10.1016/j.ymben.2015.01.005

Combining Reclaimed PET with Bio-based Monomers Enables Plastics Upcycling
journal, April 2019

Rorrer, Nicholas A.; Nicholson, Scott; Carpenter, Alberta
Joule, Vol. 3, Issue 4
DOI: 10.1016/j.joule.2019.01.018

Fungal Cellulases
journal, January 2015

Payne, Christina M.; Knott, Brandon C.; Mayes, Heather B.
Chemical Reviews, Vol. 115, Issue 3
DOI: 10.1021/cr500351c

Biotechnological upcycling of plastic waste and other non-conventional feedstocks in a circular economy
journal, April 2020

Blank, Lars Mathias; Narancic, Tanja; Mampel, Jörg
Current Opinion in Biotechnology, Vol. 62
DOI: 10.1016/j.copbio.2019.11.011

Plastic waste as a novel substrate for industrial biotechnology: Plastic waste as substrate for biotechnology
journal, August 2015

Wierckx, Nick; Prieto, M. Auxiliadora; Pomposiello, Pablo
Microbial Biotechnology, Vol. 8, Issue 6
DOI: 10.1111/1751-7915.12312

A metabolic pathway for catabolizing levulinic acid in bacteria
journal, September 2017

Rand, Jacqueline M.; Pisithkul, Tippapha; Clark, Ryan L.
Nature Microbiology, Vol. 2, Issue 12
DOI: 10.1038/s41564-017-0028-z

Outer membrane vesicles catabolize lignin-derived aromatic compounds in Pseudomonas putida KT2440
journal, April 2020

Salvachúa, Davinia; Werner, Allison Z.; Pardo, Isabel
Proceedings of the National Academy of Sciences, Vol. 117, Issue 17
DOI: 10.1073/pnas.1921073117

Production of itaconic acid from alkali pretreated lignin by dynamic two stage bioconversion
journal, April 2021

Elmore, Joshua R.; Dexter, Gara N.; Salvachúa, Davinia
Nature Communications, Vol. 12, Issue 1
DOI: 10.1038/s41467-021-22556-8

Catabolism of Benzoate and Phthalate in Rhodococcus sp. Strain RHA1: Redundancies and Convergence
journal, June 2005

Patrauchan, M. A.; Florizone, C.; Dosanjh, M.
Journal of Bacteriology, Vol. 187, Issue 12, p. 4050-4063
DOI: 10.1128/JB.187.12.4050-4063.2005

Characterization of the Terephthalate Degradation Genes of Comamonas sp. Strain E6
journal, March 2006

Sasoh, M.; Masai, E.; Ishibashi, S.
Applied and Environmental Microbiology, Vol. 72, Issue 3
DOI: 10.1128/AEM.72.3.1825-1832.2006

Identification and characterization of the AgmR regulator of Pseudomonas putida : role in alcohol utilization
journal, March 2002

Vrionis, A. Daugulis, A. Kropinski, H.
Applied Microbiology and Biotechnology, Vol. 58, Issue 4
DOI: 10.1007/s00253-001-0912-5

Bioremediation 3 . 0 : Engineering pollutant-removing bacteria in the times of systemic biology
journal, November 2017

Dvořák, Pavel; Nikel, Pablo I.; Damborský, Jiří
Biotechnology Advances, Vol. 35, Issue 7
DOI: 10.1016/j.biotechadv.2017.08.001

Gene amplification, laboratory evolution, and biosensor screening reveal MucK as a terephthalic acid transporter in Acinetobacter baylyi ADP1
journal, November 2020

Pardo, Isabel; Jha, Ramesh K.; Bermel, Ryan E.
Metabolic Engineering, Vol. 62
DOI: 10.1016/j.ymben.2020.09.009

From dirt to industrial applications: Pseudomonas putida as a Synthetic Biology chassis for hosting harsh biochemical reactions
journal, October 2016

Nikel, Pablo I.; Chavarría, Max; Danchin, Antoine
Current Opinion in Chemical Biology, Vol. 34
DOI: 10.1016/j.cbpa.2016.05.011

An engineered PET depolymerase to break down and recycle plastic bottles
journal, April 2020

Tournier, V.; Topham, C. M.; Gilles, A.
Nature, Vol. 580, Issue 7802
DOI: 10.1038/s41586-020-2149-4

Development of a high efficiency integration system and promoter library for rapid modification of Pseudomonas putida KT2440
journal, December 2017

Elmore, Joshua R.; Furches, Anna; Wolff, Gara N.
Metabolic Engineering Communications, Vol. 5
DOI: 10.1016/j.meteno.2017.04.001

Structure of the plastic-degrading Ideonella sakaiensis MHETase bound to a substrate
journal, April 2019

Palm, Gottfried J.; Reisky, Lukas; Böttcher, Dominique
Nature Communications, Vol. 10, Issue 1
DOI: 10.1038/s41467-019-09326-3

Chemical recycling of waste plastics for new materials production
journal, June 2017

Rahimi, AliReza; García, Jeannette M.
Nature Reviews Chemistry, Vol. 1, Issue 6
DOI: 10.1038/s41570-017-0046

Mechanical and chemical recycling of solid plastic waste
journal, November 2017

Ragaert, Kim; Delva, Laurens; Van Geem, Kevin
Waste Management, Vol. 69
DOI: 10.1016/j.wasman.2017.07.044

Lignin valorization through integrated biological funneling and chemical catalysis
journal, August 2014

Linger, J. G.; Vardon, D. R.; Guarnieri, M. T.
Proceedings of the National Academy of Sciences, Vol. 111, Issue 33, p. 12013-12018
DOI: 10.1073/pnas.1410657111

Ethylene Glycol Metabolism by Pseudomonas putida
journal, September 2012

Mückschel, Björn; Simon, Oliver; Klebensberger, Janosch
Applied and Environmental Microbiology, Vol. 78, Issue 24
DOI: 10.1128/AEM.02062-12

The β-Ketoadipate Pathway And The Biology Of Self-Identity
journal, October 1996

Harwood, Caroline S.; Parales, Rebecca E.
Annual Review of Microbiology, Vol. 50, Issue 1, p. 553-590
DOI: 10.1146/annurev.micro.50.1.553

A bacterium that degrades and assimilates poly(ethylene terephthalate)
journal, March 2016

Yoshida, Shosuke; Hiraga, Kazumi; Takehana, Toshihiko
Science, Vol. 351, Issue 6278
DOI: 10.1126/science.aad6359

Laboratory evolution reveals the metabolic and regulatory basis of ethylene glycol metabolism by Pseudomonas putida KT2440
journal, July 2019

Li, Wing‐Jin; Jayakody, Lahiru N.; Franden, Mary Ann
Environmental Microbiology, Vol. 21, Issue 10
DOI: 10.1111/1462-2920.14703

Bioprocess development for muconic acid production from aromatic compounds and lignin
journal, January 2018

Salvachúa, Davinia; Johnson, Christopher W.; Singer, Christine A.
Green Chemistry, Vol. 20, Issue 21
DOI: 10.1039/C8GC02519C

Genomic analysis of the aromatic catabolic pathways from Pseudomonas putida KT2440
journal, December 2002

Jimenez, Jose Ignacio; Minambres, Baltasar; Garcia, Jose Luis
Environmental Microbiology, Vol. 4, Issue 12, p. 824-841
DOI: 10.1046/j.1462-2920.2002.00370.x

Thermochemical wastewater valorization via enhanced microbial toxicity tolerance
journal, January 2018

Jayakody, Lahiru N.; Johnson, Christopher W.; Whitham, Jason M.
Energy & Environmental Science, Vol. 11, Issue 6
DOI: 10.1039/C8EE00460A

Adaptive laboratory evolution of Pseudomonas putida KT2440 improves p-coumaric and ferulic acid catabolism and tolerance
journal, December 2020

Mohamed, Elsayed T.; Werner, Allison Z.; Salvachúa, Davinia
Metabolic Engineering Communications, Vol. 11
DOI: 10.1016/j.mec.2020.e00143

Innovative Chemicals and Materials from Bacterial Aromatic Catabolic Pathways
journal, June 2019

Johnson, Christopher W.; Salvachúa, Davinia; Rorrer, Nicholas A.
Joule, Vol. 3, Issue 6
DOI: 10.1016/j.joule.2019.05.011

Up-Cycling of PET (Polyethylene Terephthalate) to the Biodegradable Plastic PHA (Polyhydroxyalkanoate)
journal, October 2008

Kenny, Shane T.; Runic, Jasmina Nikodinovic; Kaminsky, Walter
Environmental Science & Technology, Vol. 42, Issue 20
DOI: 10.1021/es801010e

Challenges and opportunities of solvent-based additive extraction methods for plastic recycling
journal, March 2020

Ügdüler, Sibel; Van Geem, Kevin M.; Roosen, Martijn
Waste Management, Vol. 104
DOI: 10.1016/j.wasman.2020.01.003

Microbial degradation of aromatic compounds — from one strategy to four
journal, October 2011

Fuchs, Georg; Boll, Matthias; Heider, Johann
Nature Reviews Microbiology, Vol. 9, Issue 11, p. 803-816
DOI: 10.1038/nrmicro2652

Manufacturing energy and greenhouse gas emissions associated with plastics consumption
journal, January 2021

Nicholson, Scott R.; Rorrer, Nicholas A.; Carpenter, Alberta C.
Joule
DOI: 10.1016/j.joule.2020.12.027

Engineering Pseudomonas putida KT2440 for efficient ethylene glycol utilization
journal, July 2018

Franden, Mary Ann; Jayakody, Lahiru N.; Li, Wing-Jin
Metabolic Engineering, Vol. 48
DOI: 10.1016/j.ymben.2018.06.003

Microbial biotechnology addressing the plastic waste disaster
journal, July 2017

Narancic, Tanja; O'Connor, Kevin E.
Microbial Biotechnology, Vol. 10, Issue 5
DOI: 10.1111/1751-7915.12775

Biological Valorization of Poly(ethylene terephthalate) Monomers for Upcycling Waste PET
journal, November 2019

Kim, Hee Taek; Kim, Jae Kyun; Cha, Hyun Gil
ACS Sustainable Chemistry & Engineering, Vol. 7, Issue 24
DOI: 10.1021/acssuschemeng.9b03908

Development of a bioprocess to convert PET derived terephthalic acid and biodiesel derived glycerol to medium chain length polyhydroxyalkanoate
journal, May 2012

Kenny, Shane T.; Runic, Jasmina Nikodinovic; Kaminsky, Walter
Applied Microbiology and Biotechnology, Vol. 95, Issue 3
DOI: 10.1007/s00253-012-4058-4

Effect of the Sb2O3 catalyst on the solid-state postpolycondensation of poly(ethylene terephthalate)
journal, January 1995

Kokkalas, Demetris E.; Bikiaris, Demetris N.; Karayannidis, George P.
Journal of Applied Polymer Science, Vol. 55, Issue 5
DOI: 10.1002/app.1995.070550516

Purification and gene cloning of the oxygenase component of the terephthalate 1,2-dioxygenase system from Delftia tsuruhatensis strain T7
journal, March 2003

Shigematsu, Toru; Yumihara, Kazuyo; Ueda, Yutaka
FEMS Microbiology Letters, Vol. 220, Issue 2
DOI: 10.1016/S0378-1097(03)00124-1

Pet Waste Management by Chemical Recycling: A Review
journal, September 2008

Sinha, Vijaykumar; Patel, Mayank R.; Patel, Jigar V.
Journal of Polymers and the Environment, Vol. 18, Issue 1
DOI: 10.1007/s10924-008-0106-7

Towards bio-upcycling of polyethylene terephthalate
journal, July 2021

Tiso, Till; Narancic, Tanja; Wei, Ren
Metabolic Engineering, Vol. 66
DOI: 10.1016/j.ymben.2021.03.011

Molecular and biochemical analysis of phthalate and terephthalate degradation by Rhodococcus sp. strain DK17
journal, November 2005

Choi, Ki Young; Kim, Dockyu; Sul, Woo Jun
FEMS Microbiology Letters, Vol. 252, Issue 2
DOI: 10.1016/j.femsle.2005.08.045

Organocatalysis for depolymerisation
journal, January 2019

Jehanno, Coralie; Pérez-Madrigal, Maria M.; Demarteau, Jeremy
Polymer Chemistry, Vol. 10, Issue 2
DOI: 10.1039/C8PY01284A

Passive membrane transport of lignin-related compounds
journal, October 2019

Vermaas, Josh V.; Dixon, Richard A.; Chen, Fang
Proceedings of the National Academy of Sciences, Vol. 116, Issue 46
DOI: 10.1073/pnas.1904643116

Plastic waste as a global challenge: are biodegradable plastics the answer to the plastic waste problem?
journal, February 2019

Narancic, Tanja; O'Connor, Kevin E.
Microbiology, Vol. 165, Issue 2
DOI: 10.1099/mic.0.000749

Novel Tripartite Aromatic Acid Transporter Essential for Terephthalate Uptake in Comamonas sp. Strain E6
journal, August 2013

Hosaka, Masaru; Kamimura, Naofumi; Toribami, Shotaro
Applied and Environmental Microbiology, Vol. 79, Issue 19
DOI: 10.1128/AEM.01600-13

Characterization and engineering of a two-enzyme system for plastics depolymerization
journal, September 2020

Knott, Brandon C.; Erickson, Erika; Allen, Mark D.
Proceedings of the National Academy of Sciences, Vol. 117, Issue 41
DOI: 10.1073/pnas.2006753117

Feeding on plastic
journal, March 2016

Bornscheuer, Uwe T.
Science, Vol. 351, Issue 6278
DOI: 10.1126/science.aaf2853

Defined Microbial Mixed Culture for Utilization of Polyurethane Monomers
journal, November 2020

Utomo, Romualdus Nugraha Catur; Li, Wing-Jin; Tiso, Till
ACS Sustainable Chemistry & Engineering, Vol. 8, Issue 47
DOI: 10.1021/acssuschemeng.0c06019

Functional Role of Lanthanides in Enzymatic Activity and Transcriptional Regulation of Pyrroloquinoline Quinone-Dependent Alcohol Dehydrogenases in Pseudomonas putida KT2440
journal, June 2017

Wehrmann, Matthias; Billard, Patrick; Martin-Meriadec, Audrey
mBio, Vol. 8, Issue 3
DOI: 10.1128/mBio.00570-17

Engineered Pseudomonas putida simultaneously catabolizes five major components of corn stover lignocellulose: Glucose, xylose, arabinose, p-coumaric acid, and acetic acid
journal, November 2020

Elmore, Joshua R.; Dexter, Gara N.; Salvachúa, Davinia
Metabolic Engineering, Vol. 62
DOI: 10.1016/j.ymben.2020.08.001

Transcriptomic Analysis Reveals a Bifurcated Terephthalate Degradation Pathway in Rhodococcus sp. Strain RHA1
journal, December 2006

Hara, Hirofumi; Eltis, Lindsay D.; Davies, Julian E.
Journal of Bacteriology, Vol. 189, Issue 5
DOI: 10.1128/JB.01322-06

One-Pot Chemo-bioprocess of PET Depolymerization and Recycling Enabled by a Biocompatible Catalyst, Betaine
journal, March 2021

Kim, Dong Hyun; Han, Dong Oh; In Shim, Kyu
ACS Catalysis, Vol. 11, Issue 7
DOI: 10.1021/acscatal.0c04014

Terephthalate 1,2-dioxygenase system from Comamonas testosteroni T-2: purification and some properties of the oxygenase component
journal, November 1994

Schläfli, H. R.; Weiss, M. A.; Leisinger, T.
Journal of Bacteriology, Vol. 176, Issue 21
DOI: 10.1128/jb.176.21.6644-6652.1994

Chemical Recycling of Poly(ethylene terephthalate)
journal, April 1997

Paszun, Daniel; Spychaj, Tadeusz
Industrial & Engineering Chemistry Research, Vol. 36, Issue 4
DOI: 10.1021/ie960563c

The revisited genome of Pseudomonas putida KT2440 enlightens its value as a robust metabolic chassis : Re-annotation of the Pseudomonas putida KT2440 genome
journal, April 2016

Belda, Eugeni; van Heck, Ruben G. A.; José Lopez-Sanchez, Maria
Environmental Microbiology, Vol. 18, Issue 10
DOI: 10.1111/1462-2920.13230

Possibilities and limitations of biotechnological plastic degradation and recycling
journal, October 2020

Wei, Ren; Tiso, Till; Bertling, Jürgen
Nature Catalysis, Vol. 3, Issue 11
DOI: 10.1038/s41929-020-00521-w

Characterization and engineering of a plastic-degrading aromatic polyesterase
journal, April 2018

Austin, Harry P.; Allen, Mark D.; Donohoe, Bryon S.
Proceedings of the National Academy of Sciences, Vol. 115, Issue 19
DOI: 10.1073/pnas.1718804115

Predicted growth in plastic waste exceeds efforts to mitigate plastic pollution
journal, September 2020

Borrelle, Stephanie B.; Ringma, Jeremy; Law, Kara Lavender
Science, Vol. 369, Issue 6510
DOI: 10.1126/science.aba3656

The PedS2/PedR2 Two-Component System Is Crucial for the Rare Earth Element Switch in Pseudomonas putida KT2440
journal, August 2018

Wehrmann, Matthias; Berthelot, Charlotte; Billard, Patrick
mSphere, Vol. 3, Issue 4
DOI: 10.1128/mSphere.00376-18

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https://doi.org/10.1002/cssc.202202277

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Title: Tandem chemical deconstruction and biological upcycling of poly(ethylene terephthalate) to β-ketoadipic acid by Pseudomonas putida KT2440

Abstract

Citation Formats

Aromatic catabolic pathway selection for optimal production of pyruvate and lactate from lignin journal, March 2015

Combining Reclaimed PET with Bio-based Monomers Enables Plastics Upcycling journal, April 2019

Fungal Cellulases journal, January 2015

Biotechnological upcycling of plastic waste and other non-conventional feedstocks in a circular economy journal, April 2020

Plastic waste as a novel substrate for industrial biotechnology: Plastic waste as substrate for biotechnology journal, August 2015

A metabolic pathway for catabolizing levulinic acid in bacteria journal, September 2017

Outer membrane vesicles catabolize lignin-derived aromatic compounds in Pseudomonas putida KT2440 journal, April 2020

Production of itaconic acid from alkali pretreated lignin by dynamic two stage bioconversion journal, April 2021

Catabolism of Benzoate and Phthalate in Rhodococcus sp. Strain RHA1: Redundancies and Convergence journal, June 2005

Characterization of the Terephthalate Degradation Genes of Comamonas sp. Strain E6 journal, March 2006

Identification and characterization of the AgmR regulator of Pseudomonas putida : role in alcohol utilization journal, March 2002

Bioremediation 3 . 0 : Engineering pollutant-removing bacteria in the times of systemic biology journal, November 2017

Gene amplification, laboratory evolution, and biosensor screening reveal MucK as a terephthalic acid transporter in Acinetobacter baylyi ADP1 journal, November 2020

From dirt to industrial applications: Pseudomonas putida as a Synthetic Biology chassis for hosting harsh biochemical reactions journal, October 2016

An engineered PET depolymerase to break down and recycle plastic bottles journal, April 2020

Development of a high efficiency integration system and promoter library for rapid modification of Pseudomonas putida KT2440 journal, December 2017

Structure of the plastic-degrading Ideonella sakaiensis MHETase bound to a substrate journal, April 2019

Chemical recycling of waste plastics for new materials production journal, June 2017

Mechanical and chemical recycling of solid plastic waste journal, November 2017

Lignin valorization through integrated biological funneling and chemical catalysis journal, August 2014

Ethylene Glycol Metabolism by Pseudomonas putida journal, September 2012

The β-Ketoadipate Pathway And The Biology Of Self-Identity journal, October 1996

A bacterium that degrades and assimilates poly(ethylene terephthalate) journal, March 2016

Laboratory evolution reveals the metabolic and regulatory basis of ethylene glycol metabolism by Pseudomonas putida KT2440 journal, July 2019

Bioprocess development for muconic acid production from aromatic compounds and lignin journal, January 2018

Genomic analysis of the aromatic catabolic pathways from Pseudomonas putida KT2440 journal, December 2002

Thermochemical wastewater valorization via enhanced microbial toxicity tolerance journal, January 2018

Adaptive laboratory evolution of Pseudomonas putida KT2440 improves p-coumaric and ferulic acid catabolism and tolerance journal, December 2020

Innovative Chemicals and Materials from Bacterial Aromatic Catabolic Pathways journal, June 2019

Up-Cycling of PET (Polyethylene Terephthalate) to the Biodegradable Plastic PHA (Polyhydroxyalkanoate) journal, October 2008

Challenges and opportunities of solvent-based additive extraction methods for plastic recycling journal, March 2020

Microbial degradation of aromatic compounds — from one strategy to four journal, October 2011

Manufacturing energy and greenhouse gas emissions associated with plastics consumption journal, January 2021

Engineering Pseudomonas putida KT2440 for efficient ethylene glycol utilization journal, July 2018

Microbial biotechnology addressing the plastic waste disaster journal, July 2017

Biological Valorization of Poly(ethylene terephthalate) Monomers for Upcycling Waste PET journal, November 2019

Development of a bioprocess to convert PET derived terephthalic acid and biodiesel derived glycerol to medium chain length polyhydroxyalkanoate journal, May 2012

Effect of the Sb2O3 catalyst on the solid-state postpolycondensation of poly(ethylene terephthalate) journal, January 1995

Purification and gene cloning of the oxygenase component of the terephthalate 1,2-dioxygenase system from Delftia tsuruhatensis strain T7 journal, March 2003

Pet Waste Management by Chemical Recycling: A Review journal, September 2008

Towards bio-upcycling of polyethylene terephthalate journal, July 2021

Molecular and biochemical analysis of phthalate and terephthalate degradation by Rhodococcus sp. strain DK17 journal, November 2005

Organocatalysis for depolymerisation journal, January 2019

Passive membrane transport of lignin-related compounds journal, October 2019

Plastic waste as a global challenge: are biodegradable plastics the answer to the plastic waste problem? journal, February 2019

Novel Tripartite Aromatic Acid Transporter Essential for Terephthalate Uptake in Comamonas sp. Strain E6 journal, August 2013

Characterization and engineering of a two-enzyme system for plastics depolymerization journal, September 2020

Feeding on plastic journal, March 2016

Defined Microbial Mixed Culture for Utilization of Polyurethane Monomers journal, November 2020

Functional Role of Lanthanides in Enzymatic Activity and Transcriptional Regulation of Pyrroloquinoline Quinone-Dependent Alcohol Dehydrogenases in Pseudomonas putida KT2440 journal, June 2017

Engineered Pseudomonas putida simultaneously catabolizes five major components of corn stover lignocellulose: Glucose, xylose, arabinose, p-coumaric acid, and acetic acid journal, November 2020

Transcriptomic Analysis Reveals a Bifurcated Terephthalate Degradation Pathway in Rhodococcus sp. Strain RHA1 journal, December 2006

One-Pot Chemo-bioprocess of PET Depolymerization and Recycling Enabled by a Biocompatible Catalyst, Betaine journal, March 2021

Terephthalate 1,2-dioxygenase system from Comamonas testosteroni T-2: purification and some properties of the oxygenase component journal, November 1994

Chemical Recycling of Poly(ethylene terephthalate) journal, April 1997

The revisited genome of Pseudomonas putida KT2440 enlightens its value as a robust metabolic chassis : Re-annotation of the Pseudomonas putida KT2440 genome journal, April 2016

Possibilities and limitations of biotechnological plastic degradation and recycling journal, October 2020

Characterization and engineering of a plastic-degrading aromatic polyesterase journal, April 2018

Predicted growth in plastic waste exceeds efforts to mitigate plastic pollution journal, September 2020

The PedS2/PedR2 Two-Component System Is Crucial for the Rare Earth Element Switch in Pseudomonas putida KT2440 journal, August 2018

Aromatic catabolic pathway selection for optimal production of pyruvate and lactate from lignin
journal, March 2015

Combining Reclaimed PET with Bio-based Monomers Enables Plastics Upcycling
journal, April 2019

Fungal Cellulases
journal, January 2015

Biotechnological upcycling of plastic waste and other non-conventional feedstocks in a circular economy
journal, April 2020

Plastic waste as a novel substrate for industrial biotechnology: Plastic waste as substrate for biotechnology
journal, August 2015

A metabolic pathway for catabolizing levulinic acid in bacteria
journal, September 2017

Outer membrane vesicles catabolize lignin-derived aromatic compounds in Pseudomonas putida KT2440
journal, April 2020

Production of itaconic acid from alkali pretreated lignin by dynamic two stage bioconversion
journal, April 2021

Catabolism of Benzoate and Phthalate in Rhodococcus sp. Strain RHA1: Redundancies and Convergence
journal, June 2005

Characterization of the Terephthalate Degradation Genes of Comamonas sp. Strain E6
journal, March 2006

Identification and characterization of the AgmR regulator of Pseudomonas putida : role in alcohol utilization
journal, March 2002

Bioremediation 3 . 0 : Engineering pollutant-removing bacteria in the times of systemic biology
journal, November 2017

Gene amplification, laboratory evolution, and biosensor screening reveal MucK as a terephthalic acid transporter in Acinetobacter baylyi ADP1
journal, November 2020

From dirt to industrial applications: Pseudomonas putida as a Synthetic Biology chassis for hosting harsh biochemical reactions
journal, October 2016

An engineered PET depolymerase to break down and recycle plastic bottles
journal, April 2020

Development of a high efficiency integration system and promoter library for rapid modification of Pseudomonas putida KT2440
journal, December 2017

Structure of the plastic-degrading Ideonella sakaiensis MHETase bound to a substrate
journal, April 2019

Chemical recycling of waste plastics for new materials production
journal, June 2017

Mechanical and chemical recycling of solid plastic waste
journal, November 2017

Lignin valorization through integrated biological funneling and chemical catalysis
journal, August 2014

Ethylene Glycol Metabolism by Pseudomonas putida
journal, September 2012

The β-Ketoadipate Pathway And The Biology Of Self-Identity
journal, October 1996

A bacterium that degrades and assimilates poly(ethylene terephthalate)
journal, March 2016

Laboratory evolution reveals the metabolic and regulatory basis of ethylene glycol metabolism by Pseudomonas putida KT2440
journal, July 2019

Bioprocess development for muconic acid production from aromatic compounds and lignin
journal, January 2018

Genomic analysis of the aromatic catabolic pathways from Pseudomonas putida KT2440
journal, December 2002

Thermochemical wastewater valorization via enhanced microbial toxicity tolerance
journal, January 2018

Adaptive laboratory evolution of Pseudomonas putida KT2440 improves p-coumaric and ferulic acid catabolism and tolerance
journal, December 2020

Innovative Chemicals and Materials from Bacterial Aromatic Catabolic Pathways
journal, June 2019

Up-Cycling of PET (Polyethylene Terephthalate) to the Biodegradable Plastic PHA (Polyhydroxyalkanoate)
journal, October 2008

Challenges and opportunities of solvent-based additive extraction methods for plastic recycling
journal, March 2020

Microbial degradation of aromatic compounds — from one strategy to four
journal, October 2011

Manufacturing energy and greenhouse gas emissions associated with plastics consumption
journal, January 2021

Engineering Pseudomonas putida KT2440 for efficient ethylene glycol utilization
journal, July 2018

Microbial biotechnology addressing the plastic waste disaster
journal, July 2017

Biological Valorization of Poly(ethylene terephthalate) Monomers for Upcycling Waste PET
journal, November 2019

Development of a bioprocess to convert PET derived terephthalic acid and biodiesel derived glycerol to medium chain length polyhydroxyalkanoate
journal, May 2012

Effect of the Sb2O3 catalyst on the solid-state postpolycondensation of poly(ethylene terephthalate)
journal, January 1995

Purification and gene cloning of the oxygenase component of the terephthalate 1,2-dioxygenase system from Delftia tsuruhatensis strain T7
journal, March 2003

Pet Waste Management by Chemical Recycling: A Review
journal, September 2008

Towards bio-upcycling of polyethylene terephthalate
journal, July 2021

Molecular and biochemical analysis of phthalate and terephthalate degradation by Rhodococcus sp. strain DK17
journal, November 2005

Organocatalysis for depolymerisation
journal, January 2019

Passive membrane transport of lignin-related compounds
journal, October 2019

Plastic waste as a global challenge: are biodegradable plastics the answer to the plastic waste problem?
journal, February 2019

Novel Tripartite Aromatic Acid Transporter Essential for Terephthalate Uptake in Comamonas sp. Strain E6
journal, August 2013

Characterization and engineering of a two-enzyme system for plastics depolymerization
journal, September 2020

Feeding on plastic
journal, March 2016

Defined Microbial Mixed Culture for Utilization of Polyurethane Monomers
journal, November 2020

Functional Role of Lanthanides in Enzymatic Activity and Transcriptional Regulation of Pyrroloquinoline Quinone-Dependent Alcohol Dehydrogenases in Pseudomonas putida KT2440
journal, June 2017

Engineered Pseudomonas putida simultaneously catabolizes five major components of corn stover lignocellulose: Glucose, xylose, arabinose, p-coumaric acid, and acetic acid
journal, November 2020

Transcriptomic Analysis Reveals a Bifurcated Terephthalate Degradation Pathway in Rhodococcus sp. Strain RHA1
journal, December 2006

One-Pot Chemo-bioprocess of PET Depolymerization and Recycling Enabled by a Biocompatible Catalyst, Betaine
journal, March 2021

Terephthalate 1,2-dioxygenase system from Comamonas testosteroni T-2: purification and some properties of the oxygenase component
journal, November 1994

Chemical Recycling of Poly(ethylene terephthalate)
journal, April 1997

The revisited genome of Pseudomonas putida KT2440 enlightens its value as a robust metabolic chassis : Re-annotation of the Pseudomonas putida KT2440 genome
journal, April 2016

Possibilities and limitations of biotechnological plastic degradation and recycling
journal, October 2020

Characterization and engineering of a plastic-degrading aromatic polyesterase
journal, April 2018

Predicted growth in plastic waste exceeds efforts to mitigate plastic pollution
journal, September 2020

The PedS2/PedR2 Two-Component System Is Crucial for the Rare Earth Element Switch in Pseudomonas putida KT2440
journal, August 2018