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Engineering unsymmetrically coordinated Cu-S1N3 single atom sites with enhanced oxygen reduction activity

Author

Listed:
  • Huishan Shang

    (School of Materials Science and Engineering, Beijing Institute of Technology)

  • Xiangyi Zhou

    (Tsinghua University)

  • Juncai Dong

    (Institute of High Energy Physics, Chinese Academy of Sciences)

  • Ang Li

    (Beijing University of Technology)

  • Xu Zhao

    (University of Science and Technology of China)

  • Qinghua Liu

    (University of Science and Technology of China)

  • Yue Lin

    (University of Science and Technology of China)

  • Jiajing Pei

    (Beijing University of Chemical Technology)

  • Zhi Li

    (Tsinghua University)

  • Zhuoli Jiang

    (School of Materials Science and Engineering, Beijing Institute of Technology)

  • Danni Zhou

    (School of Materials Science and Engineering, Beijing Institute of Technology)

  • Lirong Zheng

    (Institute of High Energy Physics, Chinese Academy of Sciences)

  • Yu Wang

    (Shanghai Institute of Applied Physics, Chinese Academy of Science)

  • Jing Zhou

    (Shanghai Institute of Applied Physics, Chinese Academy of Science)

  • Zhengkun Yang

    (University of Science and Technology of China)

  • Rui Cao

    (Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory)

  • Ritimukta Sarangi

    (Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory)

  • Tingting Sun

    (University of Science and Technology Beijing)

  • Xin Yang

    (Tsinghua University)

  • Xusheng Zheng

    (University of Science and Technology of China)

  • Wensheng Yan

    (University of Science and Technology of China)

  • Zhongbin Zhuang

    (Beijing University of Chemical Technology)

  • Jia Li

    (Tsinghua University)

  • Wenxing Chen

    (School of Materials Science and Engineering, Beijing Institute of Technology)

  • Dingsheng Wang

    (Tsinghua University)

  • Jiatao Zhang

    (School of Materials Science and Engineering, Beijing Institute of Technology)

  • Yadong Li

    (Tsinghua University)

Abstract

Atomic interface regulation is thought to be an efficient method to adjust the performance of single atom catalysts. Herein, a practical strategy was reported to rationally design single copper atoms coordinated with both sulfur and nitrogen atoms in metal-organic framework derived hierarchically porous carbon (S-Cu-ISA/SNC). The atomic interface configuration of the copper site in S-Cu-ISA/SNC is detected to be an unsymmetrically arranged Cu-S1N3 moiety. The catalyst exhibits excellent oxygen reduction reaction activity with a half-wave potential of 0.918 V vs. RHE. Additionally, through in situ X-ray absorption fine structure tests, we discover that the low-valent Cuprous-S1N3 moiety acts as an active center during the oxygen reduction process. Our discovery provides a universal scheme for the controllable synthesis and performance regulation of single metal atom catalysts toward energy applications.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-16848-8
    DOI: 10.1038/s41467-020-16848-8
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    Cited by:

    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. 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.
    3. 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.
    4. 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.
    5. 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.
    6. 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.
    7. 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.
    8. 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.
    9. 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.
    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. 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.
    12. 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.

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