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Site Activity and Population Engineering of NiRu-Layered Double Hydroxide Nanosheets Decorated with Silver Nanoparticles for Oxygen Evolution and Reduction Reactions

  • Soressa Abera Chala
    Soressa Abera Chala
    NanoElectrochemistry Laboratory, Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei 106, Taiwan
  • Meng-Che Tsai
    Meng-Che Tsai
    NanoElectrochemistry Laboratory, Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei 106, Taiwan
  • Wei-Nien Su*
    Wei-Nien Su
    NanoElectrochemistry Laboratory, Department of Applied Science and Technology, National Taiwan University of Science and Technology, Taipei 106, Taiwan
    *E-mail: [email protected]
    More by Wei-Nien Su
  • Kassa Belay Ibrahim
    Kassa Belay Ibrahim
    NanoElectrochemistry Laboratory, Department of Applied Science and Technology, National Taiwan University of Science and Technology, Taipei 106, Taiwan
  • Alemayehu Dubale Duma
    Alemayehu Dubale Duma
    NanoElectrochemistry Laboratory, Department of Applied Science and Technology, National Taiwan University of Science and Technology, Taipei 106, Taiwan
  • Min-Hsin Yeh
    Min-Hsin Yeh
    NanoElectrochemistry Laboratory, Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei 106, Taiwan
    More by Min-Hsin Yeh
  • Cheng-Yen Wen
    Cheng-Yen Wen
    Department of Material Science and Engineering, National Taiwan University, Taipei 106, Taiwan
  • Chia-Hao Yu
    Chia-Hao Yu
    Department of Material Science and Engineering, National Taiwan University, Taipei 106, Taiwan
    More by Chia-Hao Yu
  • Ting-Shan Chan
    Ting-Shan Chan
    National Synchrotron Radiation Research Center, Hsin-Chu 30076, Taiwan
  • Hongjie Dai*
    Hongjie Dai
    Department of Chemistry, Stanford University, Stanford, California 94305, United States
    *E-mail: [email protected]
    More by Hongjie Dai
  • , and 
  • Bing-Joe Hwang*
    Bing-Joe Hwang
    NanoElectrochemistry Laboratory, Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei 106, Taiwan
    National Synchrotron Radiation Research Center, Hsin-Chu 30076, Taiwan
    *E-mail: [email protected]
Cite this: ACS Catal. 2019, 9, 1, 117–129
Publication Date (Web):November 21, 2018
https://doi.org/10.1021/acscatal.8b03092
Copyright © 2018 American Chemical Society

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    Abstract

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    Developing efficient and durable bifunctional electrocatalysts for oxygen reduction and evolution reaction (ORR/OER) is highly desirable in energy conversion and storage systems. This study prepares nickel–ruthenium layered double hydroxide (NiRu-LDHs) nanosheets subjected to decoration with conductive silver nanoparticles (Ag NP/NiRu-LDHs), which interestingly induce their multivacancies associated with catalytic site activity and populations. The as-prepared Ag NP/NiRu-LDH shows excellent catalytic activity toward both OER and ORR features with low onset overpotentials of 0.21 V and −0.27 V, respectively, with a 0.76 V potential gap between OER potential at 10 mA cm–2 and ORR potential at −3 mA cm–2, demonstrating that it is the preeminent bifunctional electrocatalyst reported to date. Compared with pristine NiRu-LDHs, the resulting Ag NP/NiRu-LDHs nanosheets require only an overpotential of 0.31 V to deliver 10 mA cm–2 with excellent durability. The superb bifunctional performance of Ag NP/NiRu-LDH is ascribed to the formation of multivacancies, mutual benefits of synergistic effect between metal LDHs and silver nanoparticles, and increased accessible active sites together with site activity are the key to the perceived performance. This work provides a new strategy to decorate LDHs and to engineer multivacancies to enhance site activity and populations simultaneously as ORR/OER bifunctional electrocatalysts.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acscatal.8b03092.

    • SEM images of NiRu-LDHs at different magnification, XRD patterns of NiRu-LDHs, the table containing estimated fwhm and d-spacing of NiRu-LDHs and Ag NP/NiRu-LDHs, SEM image of Ag NPs and the corresponding UV–visible spectra, FT-IR spectra of Ag NP/NiRu-LDHs, TEM images and EDX elemental analysis of Ag NP/NiRu-LDHs, XPS spectra and the corresponding elemental compositions, fitting results of the extended XANES and FT-EXAFS of Ni K-edge for Ag NP/Ni(OH)2, NiRu-LDHs and Ag NP/NiRu-LDHs samples, Tafel plots, Nyquist plots, cyclic voltammetry curves obtained in non-Faradaic region and the derived ECSA, the table containing reported literatures and our materials for comparison, the table containing the estimated site activity and site populations (PDF)

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