IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-46739-1.html
   My bibliography  Save this article

Tailoring d-band center of high-valent metal-oxo species for pollutant removal via complete polymerization

Author

Listed:
  • Hong-Zhi Liu

    (University of Science and Technology of China)

  • Xiao-Xuan Shu

    (University of Science and Technology of China)

  • Mingjie Huang

    (University of Science and Technology of China
    Huazhong University of Science and Technology)

  • Bing-Bing Wu

    (University of Science and Technology of China)

  • Jie-Jie Chen

    (University of Science and Technology of China)

  • Xi-Sheng Wang

    (University of Science and Technology of China)

  • Hui-Lin Li

    (University of Science and Technology of China)

  • Han-Qing Yu

    (University of Science and Technology of China)

Abstract

Polymerization-driven removal of pollutants in advanced oxidation processes (AOPs) offers a sustainable way for the simultaneous achievement of contamination abatement and resource recovery, supporting a low-carbon water purification approach. However, regulating such a process remains a great challenge due to the insufficient microscopic understanding of electronic structure-dependent reaction mechanisms. Herein, this work probes the origin of catalytic pollutant polymerization using a series of transition metal (Cu, Ni, Co, and Fe) single-atom catalysts and identifies the d-band center of active site as the key driver for polymerization transfer of pollutants. The high-valent metal-oxo species, produced via peroxymonosulfate activation, are found to trigger the pollutant removal via polymerization transfer. Phenoxyl radicals, identified by the innovative spin-trapping and quenching approaches, act as the key intermediate in the polymerization reactions. More importantly, the oxidation capacity of high-valent metal-oxo species can be facilely tuned by regulating their binding strength for peroxymonosulfate through d-band center modulation. A 100% polymerization transfer ratio is achieved by lowering the d-band center. This work presents a paradigm to dynamically modulate the electronic structure of high-valent metal-oxo species and optimize pollutant removal from wastewater via polymerization.

Suggested Citation

  • Hong-Zhi Liu & Xiao-Xuan Shu & Mingjie Huang & Bing-Bing Wu & Jie-Jie Chen & Xi-Sheng Wang & Hui-Lin Li & Han-Qing Yu, 2024. "Tailoring d-band center of high-valent metal-oxo species for pollutant removal via complete polymerization," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-46739-1
    DOI: 10.1038/s41467-024-46739-1
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-46739-1
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-46739-1?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. Lu Lu & Jeremy S. Guest & Catherine A. Peters & Xiuping Zhu & Greg H. Rau & Zhiyong Jason Ren, 2018. "Wastewater treatment for carbon capture and utilization," Nature Sustainability, Nature, vol. 1(12), pages 750-758, December.
    2. Miryam Naddaf, 2023. "The world faces a water crisis — 4 powerful charts show how," Nature, Nature, vol. 615(7954), pages 774-775, March.
    3. Ying-Jie Zhang & Gui-Xiang Huang & Lea R. Winter & Jie-Jie Chen & Lili Tian & Shu-Chuan Mei & Ze Zhang & Fei Chen & Zhi-Yan Guo & Rong Ji & Ye-Zi You & Wen-Wei Li & Xian-Wei Liu & Han-Qing Yu & Menach, 2022. "Simultaneous nanocatalytic surface activation of pollutants and oxidants for highly efficient water decontamination," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    4. Lixin Wang & Longjun Rao & Maoxi Ran & Qikai Shentu & Zenglong Wu & Wenkai Song & Ziwei Zhang & Hao Li & Yuyuan Yao & Weiyang Lv & Mingyang Xing, 2023. "A polymer tethering strategy to achieve high metal loading on catalysts for Fenton reactions," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    Full references (including those not matched with items on IDEAS)

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. 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.
    2. 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.

    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. Ming-Yan Lan & Yu-Hang Li & Chong-Chen Wang & Xin-Jie Li & Jiazhen Cao & Linghui Meng & Shuai Gao & Yuhui Ma & Haodong Ji & Mingyang Xing, 2024. "Multi-channel electron transfer induced by polyvanadate in metal-organic framework for boosted peroxymonosulfate activation," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. 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.
    3. 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.
    4. Leyuan Zhang & Yucheng Zhang & Yang Liu & Sibo Wang & Calvin K. Lee & Yu Huang & Xiangfeng Duan, 2024. "High power density redox-mediated Shewanella microbial flow fuel cells," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    5. Wang, Hui & Zeng, Shufang & Pan, Xiaoli & Liu, Lei & Chen, Yunjie & Tang, Jiawei & Luo, Feng, 2022. "Bioelectrochemically assisting anaerobic digestion enhanced methane production under low-temperature," Renewable Energy, Elsevier, vol. 194(C), pages 1071-1083.
    6. Liu, Wenjie & Liu, Xingchen & Xin, Shuaishuai & Wang, Yanhao & Huo, Siyue & Fu, Wenxian & Zhao, Quanyou & Gao, Mengchun & Xie, Haijiao, 2024. "Photocatalytic fuel cell assisted by Fenton-like reaction for p-Chloronitrobenzen degradation and electricity production through S-scheme heterojunction C3N5 modified TNAs photoanode: Performance, DFT," Applied Energy, Elsevier, vol. 358(C).
    7. Zhu, Wenjing & Duan, Cuncun & Chen, Bin, 2024. "Energy efficiency assessment of wastewater treatment plants in China based on multiregional input–output analysis and data envelopment analysis," Applied Energy, Elsevier, vol. 356(C).
    8. He, Yanying & Li, Yiming & Li, Xuecheng & Liu, Yingrui & Wang, Yufen & Guo, Haixiao & Hou, Jiaqi & Zhu, Tingting & Liu, Yiwen, 2023. "Net-zero greenhouse gas emission from wastewater treatment: Mechanisms, opportunities and perspectives," Renewable and Sustainable Energy Reviews, Elsevier, vol. 184(C).
    9. Beiying Li & Conghe Liu & Jingjing Bai & Yikun Huang & Run Su & Yan Wei & Bin Ma, 2024. "Strategy to mitigate substrate inhibition in wastewater treatment systems," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    10. Zhao, Chuandang & Xu, Jiuping & Wang, Fengjuan & Xie, Guo & Tan, Cheng, 2024. "Economic–environmental trade-offs based support policy towards optimal planning of wastewater heat recovery," Applied Energy, Elsevier, vol. 364(C).
    11. Xu, Jiuping & Zhao, Chuandang & Wang, Fengjuan & Yang, Guocan, 2022. "Industrial decarbonisation oriented distributed renewable generation towards wastewater treatment sector: Case from the Yangtze River Delta region in China," Energy, Elsevier, vol. 256(C).
    12. Shenghua Wang & Dake Zhang & Wu Wang & Jun Zhong & Kai Feng & Zhiyi Wu & Boyu Du & Jiaqing He & Zhengwen Li & Le He & Wei Sun & Deren Yang & Geoffrey A. Ozin, 2022. "Grave-to-cradle upcycling of Ni from electroplating wastewater to photothermal CO2 catalysis," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    13. Ziwei Yu & Xuming Jin & Yang Guo & Qian Liu & Wenyu Xiang & Shuai Zhou & Jiaying Wang & Dailin Yang & Hao Bin Wu & Juan Wang, 2024. "Decoupled oxidation process enabled by atomically dispersed copper electrodes for in-situ chemical water treatment," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    14. Patrick Moriarty & Damon Honnery, 2023. "Review: The Energy Implications of Averting Climate Change Catastrophe," Energies, MDPI, vol. 16(17), pages 1-16, August.
    15. Qi Dang & Wei Zhang & Jiqing Liu & Liting Wang & Deli Wu & Dejin Wang & Zhendong Lei & Liang Tang, 2023. "Bias-free driven ion assisted photoelectrochemical system for sustainable wastewater treatment," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    16. Lin, Richen & O'Shea, Richard & Deng, Chen & Wu, Benteng & Murphy, Jerry D., 2021. "A perspective on the efficacy of green gas production via integration of technologies in novel cascading circular bio-systems," Renewable and Sustainable Energy Reviews, Elsevier, vol. 150(C).
    17. Ryu, Kyung Hwan & Kim, Boeun & Heo, Seongmin, 2022. "Sustainability analysis framework based on global market dynamics: A carbon capture and utilization industry case," Renewable and Sustainable Energy Reviews, Elsevier, vol. 166(C).
    18. Meng, Fanxin & Liu, Gengyuan & Liang, Sai & Su, Meirong & Yang, Zhifeng, 2019. "Critical review of the energy-water-carbon nexus in cities," Energy, Elsevier, vol. 171(C), pages 1017-1032.
    19. Xu, Ting & Song, Jianan & Lin, Weichen & Fu, Boya & Guo, Xingguo & Huang, Xia & Wu, Hui & Zhang, Xiaoyuan, 2021. "A freestanding carbon submicro fiber sponge as high-efficient bioelectrochemical anode for wastewater energy recovery and treatment," Applied Energy, Elsevier, vol. 281(C).
    20. Bong Jae Lee & Jeong Il Lee & Soo Young Yun & Cheol-Soo Lim & Young-Kwon Park, 2020. "Economic Evaluation of Carbon Capture and Utilization Applying the Technology of Mineral Carbonation at Coal-Fired Power Plant," Sustainability, MDPI, vol. 12(15), pages 1-14, July.

    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_s41467-024-46739-1. 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.