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Atomically-precise dopant-controlled single cluster catalysis for electrochemical nitrogen reduction

Author

Listed:
  • Chuanhao Yao

    (National University of Singapore
    Northwestern Polytechnical University (NPU))

  • Na Guo

    (National University of Singapore)

  • Shibo Xi

    (Institute of Chemical and Engineering Sciences)

  • Cong-Qiao Xu

    (Southern University of Science and Technology)

  • Wei Liu

    (National University of Singapore
    National University of Singapore)

  • Xiaoxu Zhao

    (National University of Singapore
    NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore
    National University of Singapore)

  • Jing Li

    (National University of Singapore)

  • Hanyan Fang

    (National University of Singapore
    National University of Singapore)

  • Jie Su

    (National University of Singapore
    National University of Singapore)

  • Zhongxin Chen

    (National University of Singapore
    NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore)

  • Huan Yan

    (National University of Singapore)

  • Zhizhan Qiu

    (National University of Singapore
    NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore)

  • Pin Lyu

    (National University of Singapore)

  • Cheng Chen

    (National University of Singapore
    NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore)

  • Haomin Xu

    (National University of Singapore
    National University of Singapore)

  • Xinnan Peng

    (National University of Singapore
    National University of Singapore)

  • Xinzhe Li

    (National University of Singapore)

  • Bin Liu

    (Nanyang Technological University)

  • Chenliang Su

    (Shenzhen University)

  • Stephen J. Pennycook

    (NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore
    National University of Singapore)

  • Cheng-Jun Sun

    (Argonne National Laboratory)

  • Jun Li

    (Southern University of Science and Technology
    Tsinghua University)

  • Chun Zhang

    (National University of Singapore
    National University of Singapore
    National University of Singapore)

  • Yonghua Du

    (Institute of Chemical and Engineering Sciences
    Brookhaven National Laboratory)

  • Jiong Lu

    (National University of Singapore
    National University of Singapore)

Abstract

The ability to precisely engineer the doping of sub-nanometer bimetallic clusters offers exciting opportunities for tailoring their catalytic performance with atomic accuracy. However, the fabrication of singly dispersed bimetallic cluster catalysts with atomic-level control of dopants has been a long-standing challenge. Herein, we report a strategy for the controllable synthesis of a precisely doped single cluster catalyst consisting of partially ligand-enveloped Au4Pt2 clusters supported on defective graphene. This creates a bimetal single cluster catalyst (Au4Pt2/G) with exceptional activity for electrochemical nitrogen (N2) reduction. Our mechanistic study reveals that each N2 molecule is activated in the confined region between cluster and graphene. The heteroatom dopant plays an indispensable role in the activation of N2 via an enhanced back donation of electrons to the N2 LUMO. Moreover, besides the heteroatom Pt, the catalytic performance of single cluster catalyst can be further tuned by using Pd in place of Pt as the dopant.

Suggested Citation

  • Chuanhao Yao & Na Guo & Shibo Xi & Cong-Qiao Xu & Wei Liu & Xiaoxu Zhao & Jing Li & Hanyan Fang & Jie Su & Zhongxin Chen & Huan Yan & Zhizhan Qiu & Pin Lyu & Cheng Chen & Haomin Xu & Xinnan Peng & Xin, 2020. "Atomically-precise dopant-controlled single cluster catalysis for electrochemical nitrogen reduction," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-18080-w
    DOI: 10.1038/s41467-020-18080-w
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    Cited by:

    1. Xin Lin & Shize Geng & Xianglong Du & Feiteng Wang & Xu Zhang & Fang Xiao & Zhengyi Xiao & Yucheng Wang & Jun Cheng & Zhifeng Zheng & Xiaoqing Huang & Lingzheng Bu, 2025. "Efficient direct formic acid electrocatalysis enabled by rare earth-doped platinum-tellurium heterostructures," Nature Communications, Nature, vol. 16(1), pages 1-14, December.

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