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    Electrostatic Stabilization of Single-Atom Catalysts by Ionic Liquids

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    Type
    Article
    Authors
    Ding, Shipeng
    Guo, Yalin
    Hülsey, Max J.
    Zhang, Bin
    Asakura, Hiroyuki
    Liu, Lingmei
    Han, Yu cc
    Gao, Min
    Hasegawa, Jun ya
    Qiao, Botao
    Zhang, Tao
    Yan, Ning
    KAUST Department
    Advanced Membranes and Porous Materials Research Center
    Chemical Science Program
    Nanostructured Functional Materials (NFM) laboratory
    Physical Science and Engineering (PSE) Division
    Date
    2019-11-04
    Online Publication Date
    2019-11-04
    Print Publication Date
    2019-12
    Embargo End Date
    2020-11-04
    Permanent link to this record
    http://hdl.handle.net/10754/660591
    
    Metadata
    Show full item record
    Abstract
    In single-atom catalysts (SACs), the isolated metal atoms on solid support are often charged. Taking advantage of this common feature, we establish ionic liquid-stabilized single-atom catalysts (ILSSACs) employing electrostatic interaction as a general stabilization strategy. While Pt nanoparticles were formed on hydroxyapatite after reaction when unprotected, Pt remained atomically dispersed on ionic liquid-stabilized samples. Density functional theory calculations reveal that the activation energy for the transformation of two isolated Pt atoms to a Pt dimer increases remarkably from 0.11 to 0.72 eV with the protection of [Bmim][BF4]. The presence of ILs also tunes the electronic state of Pt1, inducing an order-of-magnitude hydrogenation activity increase. The simple stabilization strategy is easily extended to SACs comprising various metal atom-support combinations. For instance, ILs significantly improved the stability and selectivity of a Pd1 catalyst for the hydrogenation of acetylene, thus outperforming unprotected SACs.
    Citation
    Ding, S., Guo, Y., Hülsey, M. J., Zhang, B., Asakura, H., Liu, L., … Yan, N. (2019). Electrostatic Stabilization of Single-Atom Catalysts by Ionic Liquids. Chem. doi:10.1016/j.chempr.2019.10.007
    Sponsors
    This work has been supported by the National University of Singapore Flagship Green Energy Program (#R-279-000-553-646 and R-279-000-553-731). The computations were partly performed at the Research Center for Computational Science, Okazaki, Japan, and partly supported by Grant-in-Aid for Young Scientists (B) (17K1442907) in Japan. N.Y. conceived and supervised the project. S.D. carried out the catalyst synthesis, catalytic performance test, stability evaluation, and kinetic study and conducted some characterizations. S.D. N.Y. M.H. and B.Z. analyzed the data. L.L. and Y.H. carried out the HAADF-STEM characterizations. H.A. carried out the XAS measurements and analysis. M.G. and J.H. conducted the DFT calculation. S.D. and N.Y. wrote the paper. Y.G. B.Q. and T.Z. prepared the Pd/HAP catalyst, performed the HADDF-STEM and acetylene hydrogenation measurement, and wrote the Pd/HAP section. All authors contributed to project discussions and modified the manuscript. The authors declare no competing interests.
    Publisher
    Elsevier BV
    Journal
    Chem
    DOI
    10.1016/j.chempr.2019.10.007
    Additional Links
    https://linkinghub.elsevier.com/retrieve/pii/S2451929419304619
    ae974a485f413a2113503eed53cd6c53
    10.1016/j.chempr.2019.10.007
    Scopus Count
    Collections
    Articles; Advanced Membranes and Porous Materials Research Center; Physical Science and Engineering (PSE) Division; Chemical Science Program

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