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    題名: FeMo sub-nanoclusters/single atoms for neutral ammonia electrosynthesis
    作者: Liu, Wei;Han, Lili;Wang, Hsiao-Tsu;Zhao, Xueru;Boscoboinik, J. Anibal;Liu, Xijun;Pao, Chih-Wen;Sun, Jiaqiang;Zhuo, Longchao;Luo, Jun;Ren, Junqiang;Pong, W. F.;Xin, Huolin L.
    關鍵詞: Nitrogen fixation;Ammonia electrosynthesis;Neutral electrolyte;Sub-nanocluster;Single atom;FeMo electrocatalyst
    日期: 2020-11
    上傳時間: 2021-04-15 12:11:38 (UTC+8)
    摘要: Electrochemical N2 reduction reaction (NRR) has long been regarded as a promising process to generate NH3 under ambient conditions. Therefore, developing cost-effective and high-performance non-noble-metal catalysts for NRR is highly desirable. Inspired by the biological nitrogenase structure, we here designed and synthesized a catalyst with iron-molybdenum sub-nanoclusters and single atoms on porous nitrogen-doped carbon (FeMo/NC). The catalyst features porous structure beneficial to active site exposure and accessibility to electrolyte as well as FeMo sub-nanoclusters and single atoms enabling to activate N2 molecular. In situ near-ambient pressure X-ray photoelectron spectroscopy tests reveal that during the process from vacuum to nitrogen saturation, N2 was close to, adsorbed on and interacted with Fe and Mo in FeMo/NC. The Fe and Mo through electron transfer play a key role in activating the N2 molecules. Therefore, when tested for NRR, FeMo/NC achieves the maximum Faradaic efficiency (FE) of 11.8 ± 0.8% at −0.25 V and NH3 yield rate of 26.5 ± 0.8 μg h−1 mgcat.−1 at −0.3 V in neutral electrolyte. Moreover, the catalyst exhibits ignorable variations in the FE and a slight decrease in current density for 100,000 s. This work develops a non-precious bimetallic electrocatalyst with synergetic effect capability for efficient NH3 production and provides a guideline for the design of efficient and robust catalysts with coexistence of sub-nanoclusters and single atoms.
    關聯: Nano Energy 77, 105078
    DOI: 10.1016/j.nanoen.2020.105078
    顯示於類別:[物理學系暨研究所] 期刊論文

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