IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v13y2022i1d10.1038_s41467-022-35598-3.html
   My bibliography  Save this article

Atomic design of dual-metal hetero-single-atoms for high-efficiency synthesis of natural flavones

Author

Listed:
  • Xin Zhao

    (South China University of Technology)

  • Ruiqi Fang

    (South China University of Technology)

  • Fengliang Wang

    (South China University of Technology)

  • Xiangpeng Kong

    (Harbin Institute of Technology)

  • Yingwei Li

    (South China University of Technology
    South China University of Technology–Zhuhai Institute of Modern Industrial Innovation)

Abstract

Single-atom (SA) catalysts provide extensive possibilities in pursuing fantastic catalytic performances, while their preparation still suffers from metal aggregation and pore collapsing during pyrolysis. Here we report a versatile medium-induced infiltration deposition strategy for the fabrication of SAs and hetero-SAs (MaN4/MbN4@NC; Ma = Cu, Co, Ni, Mn, Mb = Co, Cu, Fe, NC = N-doped carbon). In-situ and control experiments reveal that the catalyst fabrication relies on the “step-by-step” evolution of Ma-containing metal-organic framework (MOF) template and Mb-based metal precursor, during which molten salt acts as both pore generator in the MOF transformation, and carrier for the oriented infiltration and deposition of the latter to eventually yield metal SAs embedded on hierarchically porous support. The as-prepared hetero-SAs show excellent catalytic performances in the general synthesis of 33 kinds of natural flavones. The highly efficient synthesis is further strengthened by the reliable durability of the catalyst loaded in a flow reactor. Systematic characterizations and mechanism studies suggest that the superior catalytic performances of CuN4/CoN4@NC are attributed to the facilitated O2 activating-splitting process and significantly reduced reaction energy barriers over CoN4 due to the synergetic interactions of the adjacent CuN4.

Suggested Citation

  • Xin Zhao & Ruiqi Fang & Fengliang Wang & Xiangpeng Kong & Yingwei Li, 2022. "Atomic design of dual-metal hetero-single-atoms for high-efficiency synthesis of natural flavones," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-35598-3
    DOI: 10.1038/s41467-022-35598-3
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-022-35598-3
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-022-35598-3?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. Hongqiang Jin & Peipei Li & Peixin Cui & Jinan Shi & Wu Zhou & Xiaohu Yu & Weiguo Song & Changyan Cao, 2022. "Unprecedentedly high activity and selectivity for hydrogenation of nitroarenes with single atomic Co1-N3P1 sites," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Long Jiao & Rui Zhang & Gang Wan & Weijie Yang & Xin Wan & Hua Zhou & Jianglan Shui & Shu-Hong Yu & Hai-Long Jiang, 2020. "Nanocasting SiO2 into metal–organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
    3. Huishan Shang & Xiangyi Zhou & Juncai Dong & Ang Li & Xu Zhao & Qinghua Liu & Yue Lin & Jiajing Pei & Zhi Li & Zhuoli Jiang & Danni Zhou & Lirong Zheng & Yu Wang & Jing Zhou & Zhengkun Yang & Rui Cao , 2020. "Engineering unsymmetrically coordinated Cu-S1N3 single atom sites with enhanced oxygen reduction activity," Nature Communications, Nature, vol. 11(1), pages 1-11, 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. Jingsen Bai & Tuo Zhao & Mingjun Xu & Bingbao Mei & Liting Yang & Zhaoping Shi & Siyuan Zhu & Ying Wang & Zheng Jiang & Jin Zhao & Junjie Ge & Meiling Xiao & Changpeng Liu & Wei Xing, 2024. "Monosymmetric Fe-N4 sites enabling durable proton exchange membrane fuel cell cathode by chemical vapor modification," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Hongqiang Jin & Peipei Li & Peixin Cui & Jinan Shi & Wu Zhou & Xiaohu Yu & Weiguo Song & Changyan Cao, 2022. "Unprecedentedly high activity and selectivity for hydrogenation of nitroarenes with single atomic Co1-N3P1 sites," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    3. Meihuan Liu & Jing Zhang & Hui Su & Yaling Jiang & Wanlin Zhou & Chenyu Yang & Shuowen Bo & Jun Pan & Qinghua Liu, 2024. "In situ modulating coordination fields of single-atom cobalt catalyst for enhanced oxygen reduction reaction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    4. Hongqiang Jin & Kaixin Zhou & Ruoxi Zhang & Hongjie Cui & Yu Yu & Peixin Cui & Weiguo Song & Changyan Cao, 2023. "Regulating the electronic structure through charge redistribution in dense single-atom catalysts for enhanced alkene epoxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Shuhu Yin & Hongyuan Yi & Mengli Liu & Jian Yang & Shuangli Yang & Bin-Wei Zhang & Long Chen & Xiaoyang Cheng & Huan Huang & Rui Huang & Yanxia Jiang & Honggang Liao & Shigang Sun, 2024. "An in situ exploration of how Fe/N/C oxygen reduction catalysts evolve during synthesis under pyrolytic conditions," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    6. Yangyang Liu & Can Li & Chunhui Tan & Zengxia Pei & Tao Yang & Shuzhen Zhang & Qianwei Huang & Yihan Wang & Zheng Zhou & Xiaozhou Liao & Juncai Dong & Hao Tan & Wensheng Yan & Huajie Yin & Zhao-Qing L, 2023. "Electrosynthesis of chlorine from seawater-like solution through single-atom catalysts," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    7. Shuo Zhang & Jianghua Wu & Mengting Zheng & Xin Jin & Zihan Shen & Zhonghua Li & Yanjun Wang & Quan Wang & Xuebin Wang & Hui Wei & Jiangwei Zhang & Peng Wang & Shanqing Zhang & Liyan Yu & Lifeng Dong , 2023. "Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    8. Fangqing Wang & Peichao Zou & Yangyang Zhang & Wenli Pan & Ying Li & Limin Liang & Cong Chen & Hui Liu & Shijian Zheng, 2023. "Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    9. Li Zhang & Xiaoju Yang & Qing Yuan & Zhiming Wei & Jie Ding & Tianshu Chu & Chao Rong & Qiao Zhang & Zhenkun Ye & Fu-Zhen Xuan & Yueming Zhai & Bowei Zhang & Xuan Yang, 2023. "Elucidating the structure-stability relationship of Cu single-atom catalysts using operando surface-enhanced infrared absorption spectroscopy," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    10. Xiubei Yang & Qizheng An & Xuewen Li & Yubin Fu & Shuai Yang & Minghao Liu & Qing Xu & Gaofeng Zeng, 2024. "Charging modulation of the pyridine nitrogen of covalent organic frameworks for promoting oxygen reduction reaction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    11. Yurui Fan & Haomiao Xu & Guanqun Gao & Mingming Wang & Wenjun Huang & Lei Ma & Yancai Yao & Zan Qu & Pengfei Xie & Bin Dai & Naiqiang Yan, 2024. "Asymmetric Ru-In atomic pairs promote highly active and stable acetylene hydrochlorination," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    12. Zhimeng Tang & Lei Xu & Cheng Xie & Lirong Guo & Libo Zhang & Shenghui Guo & Jinhui Peng, 2023. "Synthesis of CuCo2S4@Expanded Graphite with crystal/amorphous heterointerface and defects for electromagnetic wave absorption," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    13. Kejun Bu & Qingyang Hu & Xiaohuan Qi & Dong Wang & Songhao Guo & Hui Luo & Tianquan Lin & Xiaofeng Guo & Qiaoshi Zeng & Yang Ding & Fuqiang Huang & Wenge Yang & Ho-Kwang Mao & Xujie Lü, 2022. "Nested order-disorder framework containing a crystalline matrix with self-filled amorphous-like innards," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    14. Juncai Dong & Yangyang Liu & Jiajing Pei & Haijing Li & Shufang Ji & Lei Shi & Yaning Zhang & Can Li & Cheng Tang & Jiangwen Liao & Shiqing Xu & Huabin Zhang & Qi Li & Shenlong Zhao, 2023. "Continuous electroproduction of formate via CO2 reduction on local symmetry-broken single-atom catalysts," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    15. Xingkun Wang & Liangliang Xu & Cheng Li & Canhui Zhang & Hanxu Yao & Ren Xu & Peixin Cui & Xusheng Zheng & Meng Gu & Jinwoo Lee & Heqing Jiang & Minghua Huang, 2023. "Developing a class of dual atom materials for multifunctional catalytic reactions," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    16. Xiao Zhou & Yuan Min & Changming Zhao & Cai Chen & Ming-Kun Ke & Shi-Lin Xu & Jie-Jie Chen & Yuen Wu & Han-Qing Yu, 2024. "Constructing sulfur and oxygen super-coordinated main-group electrocatalysts for selective and cumulative H2O2 production," Nature Communications, Nature, vol. 15(1), pages 1-13, December.

    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:13:y:2022:i:1:d:10.1038_s41467-022-35598-3. 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.