Promoting Effect of Zn in High-Loading Zn/Ni-SiO2 Catalysts for Selective Hydrogen Evolution from Methylcyclohexane Full article
| Journal |
Dalton Transactions
ISSN: 1477-9226 , E-ISSN: 1477-9234 |
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| Output data | Year: 2022, Volume: 51, Number: 15, Pages: 6068-6085 Pages count : 18 DOI: 10.1039/d2dt00332e | ||
| Tags | Binary alloys; Catalyst selectivity; High resolution transmission electron microscopy; Hydrogen; Nickel; Silica; Sol-gel process; Sol-gels; Solid solutions; Toluene; X ray absorption spectroscopy; X ray photoelectron spectroscopy; Zinc | ||
| Authors |
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| Affiliations |
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Funding (1)
| 1 | Russian Science Foundation | 19-73-20020 |
Abstract:
The dehydrogenation of methylcyclohexane to toluene was investigated over high-loading monometallic Ni-SiO2 and bimetallic Zn/Ni-SiO2 catalysts. The catalysts were prepared by the impregnation coupled with the advantageous heterophase sol–gel technique. Their performance was tested in a fixed-bed flow reactor at 250–350 °C, 0.1 MPa pressure, equimolar ratio H2/Ar (24 nL h−1 in total), and a methylcyclohexane feed rate of 12 mL h−1. Information regarding the structure of Ni–Zn catalysts was obtained by N2 and CO adsorption, temperature-programmed reduction, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, in situ X-ray diffraction, and
in situ X-ray absorption spectroscopy. The results have shown that the addition of zinc leads to the hindrance of Ni reducibility along with weakening the Ni interaction with the silica matrix. This behavior particularly indicated the formation of solid oxide nickel–zinc solutions. The catalytic properties of Zn-modified catalysts in the dehydrogenation of methylcyclohexane appeared significantly superior to their Ni–Cu counterparts. For example, the selectivity of
Zn/Ni-SiO2 catalysts toward toluene formation increased markedly with a decrease in the Ni : Zn mass ratio, achieving 97% at 350 °C over the sample with Ni : Zn = 80 : 20. This is attributed to the promoting geometric and electronic effects arising from the formation of bimetallic Ni–Zn solid solutions. Moreover, a deeper reduction of zinc and a more efficient formation of solid bimetallic solutions are observed after the catalytic tests.
Cite:
Alekseeva (Bykova) M.V.
, Gulyaeva Y.K.
, Bulavchenko O.A.
, Saraev A.A.
, Kremneva A.M.
, Stepanenko S.A.
, Koskin A.P.
, Kaichev V.V.
, Yakovlev V.A.
Promoting Effect of Zn in High-Loading Zn/Ni-SiO2 Catalysts for Selective Hydrogen Evolution from Methylcyclohexane
Dalton Transactions. 2022. V.51. N15. P.6068-6085. DOI: 10.1039/d2dt00332e WOS Scopus РИНЦ AN PMID OpenAlex
Promoting Effect of Zn in High-Loading Zn/Ni-SiO2 Catalysts for Selective Hydrogen Evolution from Methylcyclohexane
Dalton Transactions. 2022. V.51. N15. P.6068-6085. DOI: 10.1039/d2dt00332e WOS Scopus РИНЦ AN PMID OpenAlex
Dates:
| Submitted: | Feb 2, 2022 |
| Accepted: | Mar 17, 2022 |
| Published online: | Mar 17, 2022 |
| Published print: | Apr 21, 2022 |
Identifiers:
| Web of science: | WOS:000776253800001 |
| Scopus: | 2-s2.0-85128432969 |
| Elibrary: | 48429020 |
| Chemical Abstracts: | 2022:858415 |
| PMID: | 35356959 |
| OpenAlex: | W4220859987 |