IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-39201-1.html
   My bibliography  Save this article

Mechanistic studies of a lipase unveil effect of pH on hydrolysis products of small PET modules

Author

Listed:
  • Katarzyna Świderek

    (Universitat Jaume I)

  • Susana Velasco-Lozano

    (Basque Research and Technology Alliance (BRTA))

  • Miquel À. Galmés

    (Universitat Jaume I)

  • Ion Olazabal

    (University of the Basque Country UPV/EHU, Manuel de Lardizabal, 3)

  • Haritz Sardon

    (University of the Basque Country UPV/EHU, Manuel de Lardizabal, 3)

  • Fernando López-Gallego

    (Basque Research and Technology Alliance (BRTA)
    Basque Foundation for Science)

  • Vicent Moliner

    (Universitat Jaume I)

Abstract

Biocatalysis is a key technology enabling plastic recycling. However, despite advances done in the development of plastic-degrading enzymes, the molecular mechanisms that govern their catalytic performance are poorly understood, hampering the engineering of more efficient enzyme-based technologies. In this work, we study the hydrolysis of PET-derived diesters and PET trimers catalyzed by the highly promiscuous lipase B from Candida antarctica (CALB) through QM/MM molecular dynamics simulations supported by experimental Michaelis–Menten kinetics. The computational studies reveal the role of the pH on the CALB regioselectivity toward the hydrolysis of bis-(hydroxyethyl) terephthalate (BHET). We exploit this insight to perform a pH-controlled biotransformation that selectively hydrolyzes BHET to either its corresponding diacid or monoesters using both soluble and immobilized CALB. The discoveries presented here can be exploited for the valorization of BHET resulting from the organocatalytic depolymerization of PET.

Suggested Citation

  • Katarzyna Świderek & Susana Velasco-Lozano & Miquel À. Galmés & Ion Olazabal & Haritz Sardon & Fernando López-Gallego & Vicent Moliner, 2023. "Mechanistic studies of a lipase unveil effect of pH on hydrolysis products of small PET modules," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39201-1
    DOI: 10.1038/s41467-023-39201-1
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-39201-1
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-023-39201-1?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Coralie Jehanno & Jill W. Alty & Martijn Roosen & Steven Meester & Andrew P. Dove & Eugene Y.-X. Chen & Frank A. Leibfarth & Haritz Sardon, 2022. "Critical advances and future opportunities in upcycling commodity polymers," Nature, Nature, vol. 603(7903), pages 803-814, March.
    2. Hongyuan Lu & Daniel J. Diaz & Natalie J. Czarnecki & Congzhi Zhu & Wantae Kim & Raghav Shroff & Daniel J. Acosta & Bradley R. Alexander & Hannah O. Cole & Yan Zhang & Nathaniel A. Lynd & Andrew D. El, 2022. "Machine learning-aided engineering of hydrolases for PET depolymerization," Nature, Nature, vol. 604(7907), pages 662-667, April.
    3. V. Tournier & C. M. Topham & A. Gilles & B. David & C. Folgoas & E. Moya-Leclair & E. Kamionka & M.-L. Desrousseaux & H. Texier & S. Gavalda & M. Cot & E. Guémard & M. Dalibey & J. Nomme & G. Cioci & , 2020. "An engineered PET depolymerase to break down and recycle plastic bottles," Nature, Nature, vol. 580(7802), pages 216-219, April.
    4. Gottfried J. Palm & Lukas Reisky & Dominique Böttcher & Henrik Müller & Emil A. P. Michels & Miriam C. Walczak & Leona Berndt & Manfred S. Weiss & Uwe T. Bornscheuer & Gert Weber, 2019. "Structure of the plastic-degrading Ideonella sakaiensis MHETase bound to a substrate," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Teng Bao & Yuanchao Qian & Yongping Xin & James J. Collins & Ting Lu, 2023. "Engineering microbial division of labor for plastic upcycling," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    2. Zhuozhi Chen & Rongdi Duan & Yunjie Xiao & Yi Wei & Hanxiao Zhang & Xinzhao Sun & Shen Wang & Yingying Cheng & Xue Wang & Shanwei Tong & Yunxiao Yao & Cheng Zhu & Haitao Yang & Yanyan Wang & Zefang Wa, 2022. "Biodegradation of highly crystallized poly(ethylene terephthalate) through cell surface codisplay of bacterial PETase and hydrophobin," Nature Communications, Nature, vol. 13(1), pages 1-17, December.
    3. Anni Li & Yijie Sheng & Haiyang Cui & Minghui Wang & Luxuan Wu & Yibo Song & Rongrong Yang & Xiujuan Li & He Huang, 2023. "Discovery and mechanism-guided engineering of BHET hydrolases for improved PET recycling and upcycling," Nature Communications, Nature, vol. 14(1), pages 1-16, December.
    4. Jun Qi & Yadong Du & Qi Yang & Na Jiang & Jiachun Li & Yi Ma & Yangjun Ma & Xin Zhao & Jieshan Qiu, 2023. "Energy-saving and product-oriented hydrogen peroxide electrosynthesis enabled by electrochemistry pairing and product engineering," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    5. Trishnamoni Gautom & Dharmendra Dheeman & Colin Levy & Thomas Butterfield & Guadalupe Alvarez Gonzalez & Philip Roy & Lewis Caiger & Karl Fisher & Linus Johannissen & Neil Dixon, 2021. "Structural basis of terephthalate recognition by solute binding protein TphC," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
    6. Hwaseok Hong & Dongwoo Ki & Hogyun Seo & Jiyoung Park & Jaewon Jang & Kyung-Jin Kim, 2023. "Discovery and rational engineering of PET hydrolase with both mesophilic and thermophilic PET hydrolase properties," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    7. Yu Yang & Jian Min & Ting Xue & Pengcheng Jiang & Xin Liu & Rouming Peng & Jian-Wen Huang & Yingying Qu & Xian Li & Ning Ma & Fang-Chang Tsai & Longhai Dai & Qi Zhang & Yingle Liu & Chun-Chi Chen & Re, 2023. "Complete bio-degradation of poly(butylene adipate-co-terephthalate) via engineered cutinases," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    8. P. Konstantin Richter & Paula Blázquez-Sánchez & Ziyue Zhao & Felipe Engelberger & Christian Wiebeler & Georg Künze & Ronny Frank & Dana Krinke & Emanuele Frezzotti & Yuliia Lihanova & Patricia Falken, 2023. "Structure and function of the metagenomic plastic-degrading polyester hydrolase PHL7 bound to its product," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    9. Yinglu Cui & Yanchun Chen & Jinyuan Sun & Tong Zhu & Hua Pang & Chunli Li & Wen-Chao Geng & Bian Wu, 2024. "Computational redesign of a hydrolase for nearly complete PET depolymerization at industrially relevant high-solids loading," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    10. Erika Erickson & Japheth E. Gado & Luisana Avilán & Felicia Bratti & Richard K. Brizendine & Paul A. Cox & Raj Gill & Rosie Graham & Dong-Jin Kim & Gerhard König & William E. Michener & Saroj Poudel &, 2022. "Sourcing thermotolerant poly(ethylene terephthalate) hydrolase scaffolds from natural diversity," Nature Communications, Nature, vol. 13(1), pages 1-15, December.
    11. Huang, Jijiang & Veksha, Andrei & Chan, Wei Ping & Giannis, Apostolos & Lisak, Grzegorz, 2022. "Chemical recycling of plastic waste for sustainable material management: A prospective review on catalysts and processes," Renewable and Sustainable Energy Reviews, Elsevier, vol. 154(C).
    12. Yuantao Peng & Jie Yang & Chenqiang Deng & Jin Deng & Li Shen & Yao Fu, 2023. "Acetolysis of waste polyethylene terephthalate for upcycling and life-cycle assessment study," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    13. Xinlei Wei & Xue Yang & Congcong Hu & Qiangzi Li & Qianqian Liu & Yue Wu & Leipeng Xie & Xiao Ning & Fei Li & Tao Cai & Zhiguang Zhu & Yi-Heng P. Job Zhang & Yanfei Zhang & Xuejun Chen & Chun You, 2024. "ATP-free in vitro biotransformation of starch-derived maltodextrin into poly-3-hydroxybutyrate via acetyl-CoA," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    14. Elizabeth L. Bell & Gloria Rosetto & Morgan A. Ingraham & Kelsey J. Ramirez & Clarissa Lincoln & Ryan W. Clarke & Japheth E. Gado & Jacob L. Lilly & Katarzyna H. Kucharzyk & Erika Erickson & Gregg T. , 2024. "Natural diversity screening, assay development, and characterization of nylon-6 enzymatic depolymerization," Nature Communications, Nature, vol. 15(1), pages 1-17, December.
    15. Gluth, A. & Xu, Z. & Fifield, L.S. & Yang, B., 2022. "Advancing biological processing for valorization of plastic wastes," Renewable and Sustainable Energy Reviews, Elsevier, vol. 170(C).
    16. Xing-Wang Han & Xun Zhang & Youyun Zhou & Aizezi Maimaitiming & Xiu-Li Sun & Yanshan Gao & Peizhi Li & Boyu Zhu & Eugene Y.-X. Chen & Xiaokang Kuang & Yong Tang, 2024. "Circular olefin copolymers made de novo from ethylene and α-olefins," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    17. Kamali, Ali Reza & Li, Siyuan, 2023. "Molten salt-assisted valorization of waste PET plastics into nanostructured SnO2@terephthalic acid with excellent Li-ion storage performance," Applied Energy, Elsevier, vol. 334(C).
    18. Noelia Ferruz & Steffen Schmidt & Birte Höcker, 2022. "ProtGPT2 is a deep unsupervised language model for protein design," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    19. Jomin Thomas & Renuka Subhash Patil & Mahesh Patil & Jacob John, 2023. "Addressing the Sustainability Conundrums and Challenges within the Polymer Value Chain," Sustainability, MDPI, vol. 15(22), pages 1-19, November.
    20. Gustavo Bustamante & Biagio Fernando Giannetti & Feni Agostinho & Gengyuan Liu & Cecília M. V. B. Almeida, 2022. "Prioritizing Cleaner Production Actions towards Circularity: Combining LCA and Emergy in the PET Production Chain," Sustainability, MDPI, vol. 14(11), pages 1-15, June.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39201-1. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.