The H/D exchange and hydrogenolysis of propane on alumina-supported nickel catalyst

Öz, Hami

doi:10.1016/0021-9517(90)90052-l

Cited by 9 publications

(2 citation statements)

References 35 publications

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“…We monitor these two reaction steps (hydrogenolysis and rehydrogenation) using in situ 1 H and 2 H NMR spectroscopy by performing the PE hydrogenolysis reaction in pressurizable MAS reactor rotors , with a deuterated polymer ( d 4 -PE) and natural abundance hydrogen gas (Figure ). Dehydrogenation–rehydrogenation cycles lead to H/D scrambling, which is detectable by NMR through the appearance of methylene 1 H NMR signals from the PE skeleton (or through the progressive deuteration of the H 2 gas using 2 H NMR). − In contrast, a hydrogenolysis reaction leads to the appearance of methyl or methane 1 H NMR signals. These species exhibit distinct chemical shifts, which enables their independent quantification.…”

Section: Resultsmentioning

confidence: 99%

Mechanistic Insights into Processive Polyethylene Hydrogenolysis through In Situ NMR

et al. 2023

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Chemical polymer upcycling by processive catalysts is a promising plastic waste remediation strategy, with the capability of producing selective, highvalue products from waste plastics with minimal energy input. We previously designed a novel processive catalyst with a mesoporous SiO 2 shell/Pt nanoparticle/SiO 2 core architecture (mSiO 2 /Pt/SiO 2 ) that deconstructs polyolefins within narrow pores. Here, we elucidate the mechanism of processive polyolefin hydrogenolysis using in situ magic-angle spinning (MAS) nuclear magnetic resonance (NMR) spectroscopy and coarse-grained molecular dynamics simulations. We observe that most polyethylene−Pt interactions do not lead to C− C bond cleavage but rather to the release of the polymer via a dehydrogenation− rehydrogenation cycle. The porous architecture increases the likelihood that a released polymer is later cleaved and enables the catalyst to perform multiple successive cleavages to the same polymer chain. Both experiment and simulation show that the extent of processivity is strongly correlated with the length of the pores, with longer pores leading to a higher processivity.

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Section: Resultsmentioning

confidence: 99%

Mechanistic Insights into Processive Polyethylene Hydrogenolysis through In Situ NMR

et al. 2023

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“…Propane and isobutane H/D exchange over W, Rh, and Ni were later studied by Kemball. , Results were similar to that of ethane: namely, W was the most active catalyst at low temperature and showed monodeuteration, whereas Rh brought about multiple exchange to give highly deuterated products. , Activity is again measured here by the temperature required to have equal disappearance of starting alkane (not D 2 ), as the multiple exchange process requires more D . This type of measurement is therefore indicative of the first C–H bond activation and ignores secondary processes.…”

Section: H/d Exchange On Metal Catalystsmentioning

confidence: 98%

Hydrogen/Deuterium (H/D) Exchange Catalysis in Alkanes

Sattler

2018

ACS Catal.

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The catalytic exchange of hydrogen and deuterium (H/D exchange) in light alkanes has been studied for almost a century. While alkanes and their C−H bonds are relatively inert, H/D exchange studies have shown that a large number of materials can catalytically activate these bonds. These studies helped elucidate the mechanisms by which alkane C−H bonds interact with catalytic materials. This Review serves to highlight this area of research, focusing on two main classes of heterogeneous materials, metals and metal oxides, and their trends in reactivities and selectivities are described in detail. Furthermore, the ability of these materials to carry out C−H bond activation and H/D exchange catalysis is compared with that of molecular organometallic complexes, and the mechanistic relationships and similarities in these processes are proposed.

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ChemInform Abstract: The H/D Exchange and Hydrogenolysis of Propane on Alumina‐Supported Nickel Catalyst.

OEZ¹,

GAEUMANN²

1991

ChemInform

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The H/D exchange and hydrogenolysis of propane on alumina-supported nickel catalyst

Cited by 9 publications

References 35 publications

Mechanistic Insights into Processive Polyethylene Hydrogenolysis through In Situ NMR

Mechanistic Insights into Processive Polyethylene Hydrogenolysis through In Situ NMR

Hydrogen/Deuterium (H/D) Exchange Catalysis in Alkanes

ChemInform Abstract: The H/D Exchange and Hydrogenolysis of Propane on Alumina‐Supported Nickel Catalyst.

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