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  • Unsaturated p-Metal Based Metal-Organic Frameworks for Selective Nitrogen Reduction Under Ambient Conditions

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    Embargoed until: 2021-09-10
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    Accepted Manuscript (AM)
    Author(s)
    Fu, Yang
    Li, Kangkang
    Batmunkh, Munkhbayar
    Yu, Hai
    Donne, Scott W
    Jia, Baohua
    Ma, Tianyi
    Griffith University Author(s)
    Batmunkh, Munkhbayar
    Year published
    2020
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    Abstract
    Electrochemical ammonia synthesis that utilizes renewable electricity in the nitrogen reduction reaction (NRR) has recently been remarkably considered. Of particular importance is to develop efficient electrocatalysts at low costs. Herein, highly selective nitrogen capture using porous aluminum-based metal-organic frameworks (MOFs) materials, MIL-100 (Al), is first designed for the electrochemical nitrogen fixation in alkaline media under ambient conditions. Owing to the unique structure, MIL-100 (Al) exhibits remarkable NRR properties (NH3 yield: 10.6 µg h-1 cm-2 mgcat.-1, Faradaic efficiency: 22.6%) at a low overpotential ...
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    Electrochemical ammonia synthesis that utilizes renewable electricity in the nitrogen reduction reaction (NRR) has recently been remarkably considered. Of particular importance is to develop efficient electrocatalysts at low costs. Herein, highly selective nitrogen capture using porous aluminum-based metal-organic frameworks (MOFs) materials, MIL-100 (Al), is first designed for the electrochemical nitrogen fixation in alkaline media under ambient conditions. Owing to the unique structure, MIL-100 (Al) exhibits remarkable NRR properties (NH3 yield: 10.6 µg h-1 cm-2 mgcat.-1, Faradaic efficiency: 22.6%) at a low overpotential (177 mV). Investigation indicates that the catalyst shows excellent N2-selective captures due to the unsaturated metal sites binding with N2. More specifically, as Al 3p band can strongly interact with N 2p orbitals, Al as a main-group metal presents a high and selective affinity to N2. The utilization of multifunctional MOF catalysts delivers both high N2 selectivity and abundant catalytic sites, resulting in remarkable efficiency for NH3 production.
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    Journal Title
    ACS Applied Materials & Interfaces
    DOI
    https://doi.org/10.1021/acsami.0c13902
    Copyright Statement
    This document is the Postprint of a Published Work that appeared in final form in ACS Applied Materials & Interfaces, © 2020 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsami.0c13902
    Note
    This publication has been entered in Griffith Research Online as an advanced online version.
    Subject
    Chemical Sciences
    Engineering
    Publication URI
    http://hdl.handle.net/10072/397712
    Collection
    • Journal articles

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