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  • Reordering d Orbital Energies of Single‐Site Catalysts for CO2 Electroreduction

    Author(s)
    Han, Jianyu
    An, Pengfei
    Liu, Shuhu
    Zhang, Xiaofei
    Wang, Dawei
    Yuan, Yi
    Guo, Jun
    Qiu, Xueying
    Hou, Ke
    Shi, Lin
    Zhang, Yin
    Zhao, Shenlong
    Long, Chang
    Tang, Zhiyong
    Griffith University Author(s)
    Tang, Zhiyong
    Year published
    2019
    Metadata
    Show full item record
    Abstract
    The single‐site catalyst (SSC) characteristic of atomically dispersed active centers will not only maximize the catalytic activity, but also provide a promising platform for establishing the structure–activity relationship. However, arbitrary arrangements of active sites in the existed SSCs make it difficult for mechanism understanding and performance optimization. Now, a well‐defined ultrathin SSC is fabricated by assembly of metal‐porphyrin molecules, which enables the precise identification of the active sites for d‐orbital energy engineering. The activity of as‐assembled products for electrocatalytic CO2 reduction is ...
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    The single‐site catalyst (SSC) characteristic of atomically dispersed active centers will not only maximize the catalytic activity, but also provide a promising platform for establishing the structure–activity relationship. However, arbitrary arrangements of active sites in the existed SSCs make it difficult for mechanism understanding and performance optimization. Now, a well‐defined ultrathin SSC is fabricated by assembly of metal‐porphyrin molecules, which enables the precise identification of the active sites for d‐orbital energy engineering. The activity of as‐assembled products for electrocatalytic CO2 reduction is significantly promoted via lifting up the energy level of metal durn:x-wiley:14337851:media:anie201907399:anie201907399-math-0001 orbitals, exhibiting a remarkable Faradaic efficiency of 96 % at the overpotential of 500 mV. Furthermore, a turnover frequency of 4.21 s−1 is achieved with negligible decay over 48 h.
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    Journal Title
    Angewandte Chemie - International Edition
    Volume
    58
    Issue
    36
    DOI
    https://doi.org/10.1002/anie.201907399
    Subject
    Chemical sciences
    2D materials
    CO2 reduction
    electrocatalysis
    orbital reordering
    single-site catalysts
    Publication URI
    http://hdl.handle.net/10072/388113
    Collection
    • Journal articles

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