IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-47270-z.html
   My bibliography  Save this article

Upgrading CO2 to sustainable aromatics via perovskite-mediated tandem catalysis

Author

Listed:
  • Guo Tian

    (Tsinghua University)

  • Zhengwen Li

    (Tsinghua University)

  • Chenxi Zhang

    (Tsinghua University
    Ordos Laboratory
    Tsinghua University)

  • Xinyan Liu

    (University of Electronic Science and Technology of China)

  • Xiaoyu Fan

    (Tsinghua University)

  • Kui Shen

    (South China University of Technology)

  • Haibin Meng

    (Taiyuan University of Technology)

  • Ning Wang

    (Beijing University of Technology)

  • Hao Xiong

    (Tsinghua University)

  • Mingyu Zhao

    (Tsinghua University)

  • Xiaoyu Liang

    (Tsinghua University)

  • Liqiang Luo

    (Tsinghua University)

  • Lan Zhang

    (Beijing University of Technology)

  • Binhang Yan

    (Tsinghua University)

  • Xiao Chen

    (Tsinghua University
    Ordos Laboratory)

  • Hong-Jie Peng

    (University of Electronic Science and Technology of China)

  • Fei Wei

    (Tsinghua University
    Ordos Laboratory)

Abstract

The directional transformation of carbon dioxide (CO2) with renewable hydrogen into specific carbon-heavy products (C6+) of high value presents a sustainable route for net-zero chemical manufacture. However, it is still challenging to simultaneously achieve high activity and selectivity due to the unbalanced CO2 hydrogenation and C–C coupling rates on complementary active sites in a bifunctional catalyst, thus causing unexpected secondary reaction. Here we report LaFeO3 perovskite-mediated directional tandem conversion of CO2 towards heavy aromatics with high CO2 conversion (> 60%), exceptional aromatics selectivity among hydrocarbons (> 85%), and no obvious deactivation for 1000 hours. This is enabled by disentangling the CO2 hydrogenation domain from the C-C coupling domain in the tandem system for Iron-based catalyst. Unlike other active Fe oxides showing wide hydrocarbon product distribution due to carbide formation, LaFeO3 by design is endowed with superior resistance to carburization, therefore inhibiting uncontrolled C–C coupling on oxide and isolating aromatics formation in the zeolite. In-situ spectroscopic evidence and theoretical calculations reveal an oxygenate-rich surface chemistry of LaFeO3, that easily escape from the oxide surface for further precise C–C coupling inside zeolites, thus steering CO2-HCOOH/H2CO-Aromatics reaction pathway to enable a high yield of aromatics.

Suggested Citation

  • Guo Tian & Zhengwen Li & Chenxi Zhang & Xinyan Liu & Xiaoyu Fan & Kui Shen & Haibin Meng & Ning Wang & Hao Xiong & Mingyu Zhao & Xiaoyu Liang & Liqiang Luo & Lan Zhang & Binhang Yan & Xiao Chen & Hong, 2024. "Upgrading CO2 to sustainable aromatics via perovskite-mediated tandem catalysis," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47270-z
    DOI: 10.1038/s41467-024-47270-z
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-47270-z
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-47270-z?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. Cameron Hepburn & Ella Adlen & John Beddington & Emily A. Carter & Sabine Fuss & Niall Mac Dowell & Jan C. Minx & Pete Smith & Charlotte K. Williams, 2019. "The technological and economic prospects for CO2 utilization and removal," Nature, Nature, vol. 575(7781), pages 87-97, November.
    2. Yinwen Li & Wa Gao & Mi Peng & Junbo Zhang & Jialve Sun & Yao Xu & Song Hong & Xi Liu & Xingwu Liu & Min Wei & Bingsen Zhang & Ding Ma, 2020. "Interfacial Fe5C2-Cu catalysts toward low-pressure syngas conversion to long-chain alcohols," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    3. Maxim Zabilskiy & Vitaly L. Sushkevich & Dennis Palagin & Mark A. Newton & Frank Krumeich & Jeroen A. Bokhoven, 2020. "The unique interplay between copper and zinc during catalytic carbon dioxide hydrogenation to methanol," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    4. Guo Tian & Xinyan Liu & Chenxi Zhang & Xiaoyu Fan & Hao Xiong & Xiao Chen & Zhengwen Li & Binhang Yan & Lan Zhang & Ning Wang & Hong-Jie Peng & Fei Wei, 2022. "Accelerating syngas-to-aromatic conversion via spontaneously monodispersed Fe in ZnCr2O4 spinel," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    5. Zhongling Li & Wenlong Wu & Menglin Wang & Yanan Wang & Xinlong Ma & Lei Luo & Yue Chen & Kaiyuan Fan & Yang Pan & Hongliang Li & Jie Zeng, 2022. "Ambient-pressure hydrogenation of CO2 into long-chain olefins," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    6. Jian Wei & Qingjie Ge & Ruwei Yao & Zhiyong Wen & Chuanyan Fang & Lisheng Guo & Hengyong Xu & Jian Sun, 2017. "Erratum: Directly converting CO2 into a gasoline fuel," Nature Communications, Nature, vol. 8(1), pages 1-1, December.
    7. Jian Wei & Qingjie Ge & Ruwei Yao & Zhiyong Wen & Chuanyan Fang & Lisheng Guo & Hengyong Xu & Jian Sun, 2017. "Directly converting CO2 into a gasoline fuel," Nature Communications, Nature, vol. 8(1), pages 1-9, August.
    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. Jiaming Liang & Jiangtao Liu & Lisheng Guo & Wenhang Wang & Chengwei Wang & Weizhe Gao & Xiaoyu Guo & Yingluo He & Guohui Yang & Shuhei Yasuda & Bing Liang & Noritatsu Tsubaki, 2024. "CO2 hydrogenation over Fe-Co bimetallic catalysts with tunable selectivity through a graphene fencing approach," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Changjiang Hu & Zhiwen Jiang & Qunyan Wu & Shuiyan Cao & Qiuhao Li & Chong Chen & Liyong Yuan & Yunlong Wang & Wenyun Yang & Jinbo Yang & Jing Peng & Weiqun Shi & Maolin Zhai & Mehran Mostafavi & Jun , 2023. "Selective CO2 reduction to CH3OH over atomic dual-metal sites embedded in a metal-organic framework with high-energy radiation," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. Zhongling Li & Wenlong Wu & Menglin Wang & Yanan Wang & Xinlong Ma & Lei Luo & Yue Chen & Kaiyuan Fan & Yang Pan & Hongliang Li & Jie Zeng, 2022. "Ambient-pressure hydrogenation of CO2 into long-chain olefins," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    4. Sorrenti, Ilaria & Harild Rasmussen, Theis Bo & You, Shi & Wu, Qiuwei, 2022. "The role of power-to-X in hybrid renewable energy systems: A comprehensive review," Renewable and Sustainable Energy Reviews, Elsevier, vol. 165(C).
    5. Guo Tian & Xinyan Liu & Chenxi Zhang & Xiaoyu Fan & Hao Xiong & Xiao Chen & Zhengwen Li & Binhang Yan & Lan Zhang & Ning Wang & Hong-Jie Peng & Fei Wei, 2022. "Accelerating syngas-to-aromatic conversion via spontaneously monodispersed Fe in ZnCr2O4 spinel," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    6. Na Li & Bin Huang & Xue Dong & Jinsong Luo & Yi Wang & Hui Wang & Dengyun Miao & Yang Pan & Feng Jiao & Jianping Xiao & Zhenping Qu, 2022. "Bifunctional zeolites-silver catalyst enabled tandem oxidation of formaldehyde at low temperatures," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    7. Şeker, Betül & Dizaji, Azam Khodadadi & Balci, Volkan & Uzun, Alper, 2021. "MCM-41-supported tungstophosphoric acid as an acid function for dimethyl ether synthesis from CO2 hydrogenation," Renewable Energy, Elsevier, vol. 171(C), pages 47-57.
    8. Guido Busca, 2024. "Critical Aspects of Energetic Transition Technologies and the Roles of Materials Chemistry and Engineering," Energies, MDPI, vol. 17(14), pages 1-32, July.
    9. Michael Carus & Lara Dammer & Achim Raschka & Pia Skoczinski, 2020. "Renewable carbon: Key to a sustainable and future‐oriented chemical and plastic industry: Definition, strategy, measures and potential," Greenhouse Gases: Science and Technology, Blackwell Publishing, vol. 10(3), pages 488-505, June.
    10. Joey Disch & Luca Bohn & Susanne Koch & Michael Schulz & Yiyong Han & Alessandro Tengattini & Lukas Helfen & Matthias Breitwieser & Severin Vierrath, 2022. "High-resolution neutron imaging of salt precipitation and water transport in zero-gap CO2 electrolysis," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    11. Takeshi Tsuji & Masao Sorai & Masashige Shiga & Shigenori Fujikawa & Toyoki Kunitake, 2021. "Geological storage of CO2–N2–O2 mixtures produced by membrane‐based direct air capture (DAC)," Greenhouse Gases: Science and Technology, Blackwell Publishing, vol. 11(4), pages 610-618, August.
    12. Moreaux, Michel & Amigues, Jean-Pierre & van der Meijden, Gerard & Withagen, Cees, 2024. "Carbon capture: Storage vs. Utilization," Journal of Environmental Economics and Management, Elsevier, vol. 125(C).
    13. Fei Qian & Jiawei Bai & Yi Cai & Hui Yang & Xue-Min Cao & Xingchen Liu & Xing-Wu Liu & Yong Yang & Yong-Wang Li & Ding Ma & Xiao-Dong Wen, 2024. "Stabilized ε-Fe2C catalyst with Mn tuning to suppress C1 byproduct selectivity for high-temperature olefin synthesis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    14. Tihamér Tibor Sebestyén, 2024. "Evaluation of the Carbon Footprint of Wooden Glamping Structures by Life Cycle Assessment," Sustainability, MDPI, vol. 16(7), pages 1-27, March.
    15. Xuemei Wu & Chengwei Wang & Shengying Zhao & Yang Wang & Tao Zhang & Jie Yao & Weizhe Gao & Baizhang Zhang & Taiki Arakawa & Yingluo He & Fei Chen & Minghui Tan & Guohui Yang & Noritatsu Tsubaki, 2024. "Dual-engine-driven realizing high-yield synthesis of Para-Xylene directly from CO2-containing syngas," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    16. Georgios Varvoutis & Athanasios Lampropoulos & Evridiki Mandela & Michalis Konsolakis & George E. Marnellos, 2022. "Recent Advances on CO 2 Mitigation Technologies: On the Role of Hydrogenation Route via Green H 2," Energies, MDPI, vol. 15(13), pages 1-38, June.
    17. Tuğçe Beyazay & Kendra S. Belthle & Christophe Farès & Martina Preiner & Joseph Moran & William F. Martin & Harun Tüysüz, 2023. "Ambient temperature CO2 fixation to pyruvate and subsequently to citramalate over iron and nickel nanoparticles," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    18. Subrato Acharjya & Jiacheng Chen & Minghui Zhu & Chong Peng, 2021. "Elucidating the reactivity and nature of active sites for tin phthalocyanine during CO2 reduction," Greenhouse Gases: Science and Technology, Blackwell Publishing, vol. 11(6), pages 1191-1197, December.
    19. TsingHai Wang & Cheng-Di Dong & Jui-Yen Lin & Chiu-Wen Chen & Jo-Shu Chang & Hyunook Kim & Chin-Pao Huang & Chang-Mao Hung, 2021. "Recent Advances in Carbon Dioxide Conversion: A Circular Bioeconomy Perspective," Sustainability, MDPI, vol. 13(12), pages 1-31, June.
    20. Chang, Yuan & Gao, Siqi & Ma, Qian & Wei, Ying & Li, Guoping, 2024. "Techno-economic analysis of carbon capture and utilization technologies and implications for China," Renewable and Sustainable Energy Reviews, Elsevier, vol. 199(C).

    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_s41467-024-47270-z. 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.