IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-45106-4.html
   My bibliography  Save this article

Nanoconfinement-triggered oligomerization pathway for efficient removal of phenolic pollutants via a Fenton-like reaction

Author

Listed:
  • Xiang Zhang

    (Nanjing University of Science and Technology)

  • Jingjing Tang

    (Nanjing University of Science and Technology)

  • Lingling Wang

    (Nanjing University of Science and Technology)

  • Chuan Wang

    (Nanjing University of Science and Technology)

  • Lei Chen

    (Nanjing University)

  • Xinqing Chen

    (Chinese Academy of Sciences)

  • Jieshu Qian

    (Nanjing University of Science and Technology
    Nanjing University
    Wuxi University)

  • Bingcai Pan

    (Nanjing University)

Abstract

Heterogeneous Fenton reaction represents one of the most reliable technologies to ensure water safety, but is currently challenged by the sluggish Fe(III) reduction, excessive input of chemicals for organic mineralization, and undesirable carbon emission. Current endeavors to improve the catalytic performance of Fenton reaction are mostly focused on how to accelerate Fe(III) reduction, while the pollutant degradation step is habitually overlooked. Here, we report a nanoconfinement strategy by using graphene aerogel (GA) to support UiO-66-NH2-(Zr) binding atomic Fe(III), which alters the carbon transfer route during phenol removal from kinetically favored ring-opening route to thermodynamically favored oligomerization route. GA nanoconfinement favors the Fe(III) reduction by enriching the reductive intermediates and allows much faster phenol removal than the unconfined analog (by 208 times in terms of first-order rate constant) and highly efficient removal of total organic carbon, i.e., 92.2 ± 3.7% versus 3.6 ± 0.3% in 60 min. Moreover, this oligomerization route reduces the oxidant consumption for phenol removal by more than 95% and carbon emission by 77.9%, compared to the mineralization route in homogeneous Fe2++H2O2 system. Our findings may upgrade the regulatory toolkit for Fenton reactions and provide an alternative carbon transfer route for the removal of aqueous pollutants.

Suggested Citation

  • Xiang Zhang & Jingjing Tang & Lingling Wang & Chuan Wang & Lei Chen & Xinqing Chen & Jieshu Qian & Bingcai Pan, 2024. "Nanoconfinement-triggered oligomerization pathway for efficient removal of phenolic pollutants via a Fenton-like reaction," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45106-4
    DOI: 10.1038/s41467-024-45106-4
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-45106-4
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-45106-4?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. Tongcai Liu & Shaoze Xiao & Nan Li & Jiabin Chen & Xuefei Zhou & Yajie Qian & Ching-Hua Huang & Yalei Zhang, 2023. "Water decontamination via nonradical process by nanoconfined Fenton-like catalysts," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Kuntal Manna & Pengfei Ji & Zekai Lin & Francis X. Greene & Ania Urban & Nathan C. Thacker & Wenbin Lin, 2016. "Chemoselective single-site Earth-abundant metal catalysts at metal–organic framework nodes," Nature Communications, Nature, vol. 7(1), pages 1-11, November.
    3. Chongqing Yang & Renhao Dong & Mao Wang & Petko St. Petkov & Zhitao Zhang & Mingchao Wang & Peng Han & Marco Ballabio & Sascha A. Bräuninger & Zhongquan Liao & Jichao Zhang & Friedrich Schwotzer & Ehr, 2019. "A semiconducting layered metal-organic framework magnet," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    4. Katherine A. Henzler-Wildman & Vu Thai & Ming Lei & Maria Ott & Magnus Wolf-Watz & Tim Fenn & Ed Pozharski & Mark A. Wilson & Gregory A. Petsko & Martin Karplus & Christian G. Hübner & Dorothee Kern, 2007. "Intrinsic motions along an enzymatic reaction trajectory," Nature, Nature, vol. 450(7171), pages 838-844, December.
    5. Xu Qiu & Yueqian Sang & Hao Wu & Xiao-Song Xue & Zixi Yan & Yachong Wang & Zengrui Cheng & Xiaoyang Wang & Hui Tan & Song Song & Guisheng Zhang & Xiaohui Zhang & K. N. Houk & Ning Jiao, 2021. "Cleaving arene rings for acyclic alkenylnitrile synthesis," Nature, Nature, vol. 597(7874), pages 64-69, September.
    6. Changxia Li & Jin Yang & Pradip Pachfule & Shuang Li & Meng-Yang Ye & Johannes Schmidt & Arne Thomas, 2020. "Ultralight covalent organic framework/graphene aerogels with hierarchical porosity," Nature Communications, Nature, vol. 11(1), pages 1-8, 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. Nicolas Palopoli & Alexander Miguel Monzon & Gustavo Parisi & Maria Silvina Fornasari, 2016. "Addressing the Role of Conformational Diversity in Protein Structure Prediction," PLOS ONE, Public Library of Science, vol. 11(5), pages 1-14, May.
    2. Dilek Eren & Burak Alakent, 2013. "Frequency Response of a Protein to Local Conformational Perturbations," PLOS Computational Biology, Public Library of Science, vol. 9(9), pages 1-15, September.
    3. Sihua Feng & Hengli Duan & Hao Tan & Fengchun Hu & Chaocheng Liu & Yao Wang & Zhi Li & Liang Cai & Yuyang Cao & Chao Wang & Zeming Qi & Li Song & Xuguang Liu & Zhihu Sun & Wensheng Yan, 2023. "Intrinsic room-temperature ferromagnetism in a two-dimensional semiconducting metal-organic framework," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Weijun Weng & Jia Guo, 2022. "The effect of enantioselective chiral covalent organic frameworks and cysteine sacrificial donors on photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    5. Chengsen Cui & Lu-Jia Yang & Zi-Wei Liu & Xian Shu & Wei-Wei Zhang & Yuan Gao & Yu-Xuan Wang & Te Wang & Chun-Chi Chen & Rey-Ting Guo & Shu-Shan Gao, 2024. "Substrate specificity of a branch of aromatic dioxygenases determined by three distinct motifs," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    6. Xiao-Li Xu & Nian-Nian Wang & Yong-Hao Zou & Xiao Qin & Peng Wang & Xiang-Yu Lu & Xiao-Yu Zhang & Wei-Yin Sun & Yi Lu, 2024. "N, N’-bidentate ligand anchored palladium catalysts on MOFs for efficient Heck reaction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    7. Kit-Ying Chan & Xi Shen & Jie Yang & Keng-Te Lin & Harun Venkatesan & Eunyoung Kim & Heng Zhang & Jeng-Hun Lee & Jinhong Yu & Jinglei Yang & Jang-Kyo Kim, 2022. "Scalable anisotropic cooling aerogels by additive freeze-casting," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    8. Xiang Gao & Zhichao Yang & Wen Zhang & Bingcai Pan, 2024. "Carbon redirection via tunable Fenton-like reactions under nanoconfinement toward sustainable water treatment," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    9. Shu-Yan Jiang & Zhi-Bei Zhou & Shi-Xian Gan & Ya Lu & Chao Liu & Qiao-Yan Qi & Jin Yao & Xin Zhao, 2024. "Creating amphiphilic porosity in two-dimensional covalent organic frameworks via steric-hindrance-mediated precision hydrophilic-hydrophobic microphase separation," Nature Communications, Nature, vol. 15(1), pages 1-7, December.
    10. Santiago Esteban-Martín & Robert Bryn Fenwick & Jörgen Ådén & Benjamin Cossins & Carlos W Bertoncini & Victor Guallar & Magnus Wolf-Watz & Xavier Salvatella, 2014. "Correlated Inter-Domain Motions in Adenylate Kinase," PLOS Computational Biology, Public Library of Science, vol. 10(7), pages 1-7, July.
    11. Gregory D Friedland & Nils-Alexander Lakomek & Christian Griesinger & Jens Meiler & Tanja Kortemme, 2009. "A Correspondence Between Solution-State Dynamics of an Individual Protein and the Sequence and Conformational Diversity of its Family," PLOS Computational Biology, Public Library of Science, vol. 5(5), pages 1-16, May.
    12. Lei Zhang & Hanwen Liu & Bo Song & Jialun Gu & Lanxi Li & Wenhui Shi & Gan Li & Shiyu Zhong & Hui Liu & Xiaobo Wang & Junxiang Fan & Zhi Zhang & Pengfei Wang & Yonggang Yao & Yusheng Shi & Jian Lu, 2024. "Wood-inspired metamaterial catalyst for robust and high-throughput water purification," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    13. Robert Peach & Alexis Arnaudon & Mauricio Barahona, 2022. "Relative, local and global dimension in complex networks," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    14. Panagiota Perlepe & Itziar Oyarzabal & Laura Voigt & Mariusz Kubus & Daniel N. Woodruff & Sebastian E. Reyes-Lillo & Michael L. Aubrey & Philippe Négrier & Mathieu Rouzières & Fabrice Wilhelm & Andrei, 2022. "From an antiferromagnetic insulator to a strongly correlated metal in square-lattice MCl2(pyrazine)2 coordination solids," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    15. Zelin Wu & Zhaokun Xiong & Bingkun Huang & Gang Yao & Sihui Zhan & Bo Lai, 2024. "Long-range interactions driving neighboring Fe–N4 sites in Fenton-like reactions for sustainable water decontamination," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    16. Sebastian L B König & Mélodie Hadzic & Erica Fiorini & Richard Börner & Danny Kowerko & Wolf U Blanckenhorn & Roland K O Sigel, 2013. "BOBA FRET: Bootstrap-Based Analysis of Single-Molecule FRET Data," PLOS ONE, Public Library of Science, vol. 8(12), pages 1-17, December.
    17. Ruijie Xie & Kaiheng Guo & Yong Li & Yingguang Zhang & Huanran Zhong & Dennis Y. C. Leung & Haibao Huang, 2024. "Harnessing air-water interface to generate interfacial ROS for ultrafast environmental remediation," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    18. Yan Meng & Yu-Qin Liu & Chao Wang & Yang Si & Yun-Jie Wang & Wen-Qi Xia & Tian Liu & Xu Cao & Zhi-Yan Guo & Jie-Jie Chen & Wen-Wei Li, 2024. "Nanoconfinement steers nonradical pathway transition in single atom fenton-like catalysis for improving oxidant utilization," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    19. Kai Wang & Shiyang Long & Pu Tian, 2015. "Hierarchical Conformational Analysis of Native Lysozyme Based on Sub-Millisecond Molecular Dynamics Simulations," PLOS ONE, Public Library of Science, vol. 10(6), pages 1-17, June.
    20. Fabian Paul & Thomas R Weikl, 2016. "How to Distinguish Conformational Selection and Induced Fit Based on Chemical Relaxation Rates," PLOS Computational Biology, Public Library of Science, vol. 12(9), pages 1-17, September.

    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:15:y:2024:i:1:d:10.1038_s41467-024-45106-4. 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.