Investigating the effect of metal nuclearity on activity for ethylene hydrogenation by metal-organic-framework-supported oxy-Ni(II) catalysts

Wang, Qining; Pengmei, Zihan; Pandharkar, Riddhish; Gagliardi, Laura; Hupp, Joseph T.; Notestein, Justin M.

doi:10.1016/j.jcat.2022.01.033

Investigating the effect of metal nuclearity on activity for ethylene hydrogenation by metal-organic-framework-supported oxy-Ni(II) catalysts

Journal Article · Fri Feb 04 04:00:00 EST 2022 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2022.01.033· OSTI ID:1909339

Wang, Qining ^[1]; Pengmei, Zihan ^[2]; Pandharkar, Riddhish ^[2]; Gagliardi, Laura ^[3]; Hupp, Joseph T. ^[1]; Notestein, Justin M. ^[1]

Northwestern Univ., Evanston, IL (United States)
Univ. of Chicago, IL (United States)
Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)

Metal-organic frameworks (MOFs), thanks to their well-defined coordination sites, are promising for studying catalytically active structures. Here, to understand the effect of metal nuclearity in MOF-supported catalysts, we adjusted the nuclearity of oxy-Ni(II) supported on the zirconia-like nodes of MOF NU-1000 by modulating the Ni loading, where the organic linkers served to prevent node-to-node migration of grafted nickel ions. At the single-node level, we grafted auxiliary structural linkers, naphthalene dicarboxylate, to reduce the number of binding/grafting sites. We found higher catalytic rates at higher Ni loading for ethylene hydrogenation on a per-nickel-ion basis, despite the similar chemical environment of Ni(II) at different loadings; catalysts consisting mainly of pairs of nickel ions were more reactive than those of single nickel ions. These observations illustrate the need for at least two proximal nickel ions for effective catalysis – presumably one for hydrogen binding and heterolytic splitting and one for ethylene binding and activation.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Northwestern University; National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357; SC0012702; FG02-03ER15457; SC0001329

OSTI ID:: 1909339

Alternate ID(s):: OSTI ID: 1855428
OSTI ID: 1856400
OSTI ID: 2482301

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Vol. 407; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Active sites
Catalyst nuclearity
Ethylene hydrogenation
MOFs
Metal-organic frameworks
Nickel catalysts

Investigating the effect of metal nuclearity on activity for ethylene hydrogenation by metal-organic-framework-supported oxy-Ni(II) catalysts

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