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Identification of Active Sites for Ammonia Electrosynthesis on Ruthenium

  • Lin Hu
    Lin Hu
    Department of Materials Science and Engineering, University of Central Florida, Orlando, Florida32816, United States
    More by Lin Hu
  • Hemanth Somarajan Pillai
    Hemanth Somarajan Pillai
    Department of Chemical Engineering, Virginia Polytechnic Institute and State University, Blacksburg, Virginia24061, United States
  • Corbin Feit
    Corbin Feit
    Department of Materials Science and Engineering, University of Central Florida, Orlando, Florida32816, United States
    More by Corbin Feit
  • Kaige Shi
    Kaige Shi
    Department of Physics, University of Central Florida, Orlando, Florida32816, United States
    More by Kaige Shi
  • Zhengning Gao
    Zhengning Gao
    Department of Materials Science and Engineering, University of Central Florida, Orlando, Florida32816, United States
  • Parag Banerjee*
    Parag Banerjee
    Department of Materials Science and Engineering, University of Central Florida, Orlando, Florida32816, United States
    Renewable Energy and Chemical Transformations (REACT) Cluster, University of Central Florida, Orlando, Florida32816, United States
    NanoScience and Technology Center, University of Central Florida, Orlando, Florida32816, United States
    Florida Solar Energy Center, University of Central Florida, Orlando, Florida32816, United States
    *P.B.: email, [email protected]
  • Hongliang Xin*
    Hongliang Xin
    Department of Chemical Engineering, Virginia Polytechnic Institute and State University, Blacksburg, Virginia24061, United States
    *H.X.: email, [email protected]
  • , and 
  • Xiaofeng Feng*
    Xiaofeng Feng
    Department of Materials Science and Engineering, University of Central Florida, Orlando, Florida32816, United States
    Department of Physics, University of Central Florida, Orlando, Florida32816, United States
    Renewable Energy and Chemical Transformations (REACT) Cluster, University of Central Florida, Orlando, Florida32816, United States
    NanoScience and Technology Center, University of Central Florida, Orlando, Florida32816, United States
    Department of Chemistry, University of Central Florida, Orlando, Florida32816, United States
    *X.F.: email, [email protected]
Cite this: ACS Energy Lett. 2022, 7, 12, 4290–4298
Publication Date (Web):November 4, 2022
https://doi.org/10.1021/acsenergylett.2c02175
Copyright © 2022 American Chemical Society

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    Abstract

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    Electrochemical N2 reduction reaction (NRR) provides an attractive approach toward sustainable NH3 production, while the design of electrocatalysts for NRR is hindered by the lack of knowledge of the structure–activity relationships and active sites. Here we report a prominent size-dependent activity for the NRR on Ru nanoparticles prepared by atomic layer deposition. As the Ru particle size increased from 2.1 to 8.4 nm, the mass activity and Faradaic efficiency for NH3 production both decreased monotonically, while the specific (Ru-surface-area-normalized) activity reached the highest value on 3.8 nm Ru nanoparticles but declined by 5-fold on 8.4 nm Ru nanoparticles. Density functional theory (DFT) calculations and free energy analysis of elementary steps revealed the Ru D5 step site, with its maximal population at ∼4 nm particles, as the active site for the NRR on Ru, because it favors the adsorption of the *N2H intermediate compared to other surface sites while not getting poisoned by the *NH2 intermediate.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.2c02175.

    • Experimental methods, additional materials characterization data, electrochemical data, and DFT calculation results (Figures S1–S15) (PDF)

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    Cited By

    This article is cited by 6 publications.

    1. Zhengyao He, Yiqun Chen, Jingyi Tian, Xueyi Cheng, Minqi Xia, Cao Zhou, Yan Zhang, Xizhang Wang, Lijun Yang, Qiang Wu, Zheng Hu. Highly Dispersed Quasi-1 nm Ruthenium Nanoclusters on Hierarchical Nitrogen-Doped Carbon Nanocages Constructed by Surface-Constrained Sintering for Alkaline Hydrogen Evolution. ACS Applied Nano Materials 2024, 7 (10) , 11882-11889. https://doi.org/10.1021/acsanm.4c01438
    2. Huijiao Wang, Gening Du, Jinzhi Jia, Junfeng Huang, Mudong Tu, Jinhua Zhang, Yong Peng, Hua Li, Cailing Xu. Ru-Doped NiFe-MIL-53 with Facilitated Reconstruction and Active Hydrogen Supplement for Enhanced Nitrate Reduction. Inorganic Chemistry 2024, 63 (20) , 9212-9220. https://doi.org/10.1021/acs.inorgchem.4c00766
    3. Naoki Kamitani, SeongWoo Jeong, Hiroki Habazaki, Yoshitaka Aoki. Vanadium Nitride Is an Efficient Hydrogen-Diffusive Cathode for Green Ammonia Electrochemical Synthesis by Protonic Solid Oxide Electrolysis Cells. ACS Sustainable Chemistry & Engineering 2024, 12 (5) , 2100-2109. https://doi.org/10.1021/acssuschemeng.3c07736
    4. Kaige Shi, Maia D. Willis, Zhuanghe Ren, Xiaofeng Feng. Efficient Recycling of Dilute Nitrate to Ammonia Using Cu Nanowire Electrocatalyst. The Journal of Physical Chemistry C 2023, 127 (42) , 20710-20717. https://doi.org/10.1021/acs.jpcc.3c05804
    5. Du San Baek, Hyeong Yong Lim, Jinjong Kim, Jinyoung Lee, June Sung Lim, Dayeon Kim, Jong Hoon Lee, Ji-Wook Jang, Sang Kyu Kwak, Sang Hoon Joo. Volcanic-Size-Dependent Activity Trends in Ru-Catalyzed Alkaline Hydrogen Evolution Reaction. ACS Catalysis 2023, 13 (20) , 13638-13649. https://doi.org/10.1021/acscatal.3c02560
    6. Zhuanghe Ren, Kaige Shi, Xiaofeng Feng. Elucidating the Intrinsic Activity and Selectivity of Cu for Nitrate Electroreduction. ACS Energy Letters 2023, 8 (9) , 3658-3665. https://doi.org/10.1021/acsenergylett.3c01226