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  1. Article ; Online: Methane-H

    Wang, Yong / Zhao, Wenru / Chen, Xiaofeng / Ji, Yinjie / Zhu, Xilei / Chen, Xiaomai / Mei, Donghai / Shi, Hui / Lercher, Johannes A

    Journal of the American Chemical Society

    2024  Volume 146, Issue 12, Page(s) 8630–8640

    Abstract: ... ...

    Abstract H
    Language English
    Publishing date 2024-03-15
    Publishing country United States
    Document type Journal Article
    ZDB-ID 3155-0
    ISSN 1520-5126 ; 0002-7863
    ISSN (online) 1520-5126
    ISSN 0002-7863
    DOI 10.1021/jacs.4c00738
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article: On the multifaceted roles of NiSx in hydrodearomatization reactions catalyzed by unsupported Ni-promoted MoS2

    Vogelgsang, Ferdinand / Ji, Yinjie / Shi, Hui / Lercher, Johannes A

    Journal of catalysis. 2020 Nov., v. 391

    2020  

    Abstract: A series of unsupported Ni-Mo sulfide catalysts with varying Ni contents (0.13–0.72 molNᵢ molNᵢ₊Mₒ⁻¹) was post-synthetically treated with concentrated HCl to remove large crystallites of accessible NiSₓ. These sulfide particles inevitably form and grow ... ...

    Abstract A series of unsupported Ni-Mo sulfide catalysts with varying Ni contents (0.13–0.72 molNᵢ molNᵢ₊Mₒ⁻¹) was post-synthetically treated with concentrated HCl to remove large crystallites of accessible NiSₓ. These sulfide particles inevitably form and grow at Ni concentrations required for the synthesis, but generally have very low activities. In all cases, Ni concentrations were greatly reduced by the HCl treatment. While this ‘leaching’ strategy successfully improved the reaction rates of high Ni-content (>0.4 molNᵢ molₘₑₜₐₗ⁻¹) catalysts for the hydrogenation of phenanthrene, modest to drastic decreases in catalytic rates (×0.1–0.8) were registered for catalysts with lower Ni concentrations. For the lowest Ni-loaded catalyst (0.05 molNᵢ molₘₑₜₐₗ⁻¹), HCl treatment caused a dramatic loss of specific surface area and catalytic activity by more than a factor of 6 and shifted the selectivity pattern to that of pure MoS₂. These observations allow us to conclude that Ni atoms incorporated at the slab edges are inherently susceptible to HCl attack. NiSₓ, however, are the preferential sites at which HCl induces dissolution. Experiments with inter-particle mixtures and segregated beds of NiSₓ and MoS₂ demonstrate that NiSₓ not only activates H₂, but also acts as a reservoir to dynamically incorporate Ni in the MoS₂ slabs at reaction conditions. These beneficial effects are reduced, as nickel sulfide particles become excessively abundant as typical for high Ni-content catalysts, for which edge substitution by Ni is near or at its maximum. The areal activity and concentration of chemisorbed nitric oxide (NO) are well correlated for the leached catalysts, with the exception of the lowest Ni-containing catalyst that has a low degree of Ni edge substitution (<20% of total edge atoms) and predominantly unpromoted sites. This linear correlation shows that the Ni-promoted sites are more than five-fold as active as the unpromoted sites.
    Keywords catalysts ; catalytic activity ; correlation ; crystallites ; exhibitions ; hydrogenation ; leaching ; mixtures ; nickel ; nitric oxide ; particles ; phenanthrenes ; slabs ; sulfides ; surface area ; synthesis
    Language English
    Dates of publication 2020-11
    Size p. 212-223.
    Publishing place Elsevier Inc.
    Document type Article
    Note NAL-light
    ZDB-ID 1468993-5
    ISSN 1090-2694 ; 0021-9517
    ISSN (online) 1090-2694
    ISSN 0021-9517
    DOI 10.1016/j.jcat.2020.08.026
    Database NAL-Catalogue (AGRICOLA)

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