Structure-activity relationship in hydrogenolysis of polyolefins over Ru/support catalysts

Tamura, Masazumi; Miyaoka, Shuhei; Nakaji, Yosuke; Tanji, Mifumi; Kumagai, Seiji; Nakagawa, Yoshinao; Yoshioka, Toshiaki; Tomishige, Keiichi

doi:10.1016/j.apcatb.2022.121870

Cited by 58 publications

(55 citation statements)

References 37 publications

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“…Later, the same group discovered that the Ru/ZrO 2 catalyst shows higher activity than Ru/CeO 2 . 53 The structure–performance study showed a volcano correlation between the PE conversion and the Ru particle size (1–9 nm), and the highest PE conversion can be achieved at ∼2.5 nm Ru particle size. The selectivity towards gaseous products is low at medium to small Ru particle sizes (1–7 nm), but high at large Ru particles (>7 nm).…”

Section: Catalytic Hydroconversion Processes For Deconstruction Of Po...mentioning

confidence: 92%

“…Pt- and Ru-based catalysts are predominantly used in the hydrogenolysis of polyolefins. 40–47 The supports used are usually non-acidic materials, such as carbon materials, 40,48–51 CeO 2 , 52–54 TiO 2 , 55,56 SrTiO 3 , 47 ZrO 2 (ref. 53) and so on.…”

Section: Catalytic Hydroconversion Processes For Deconstruction Of Po...mentioning

confidence: 99%

“…40–47 The supports used are usually non-acidic materials, such as carbon materials, 40,48–51 CeO 2 , 52–54 TiO 2 , 55,56 SrTiO 3 , 47 ZrO 2 (ref. 53) and so on. Unlike the hydrocracking reaction, the metal surface is the only active site for both C–H bond activation and C–C bond breaking in polyolefins, whereas no isomerization reaction occurs due to the lack of acidic sites and linear alkanes are formed as the main products from PE hydrogenolysis.…”

Section: Catalytic Hydroconversion Processes For Deconstruction Of Po...mentioning

confidence: 99%

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Catalytic hydroconversion processes for upcycling plastic waste to fuels and chemicals

Wei¹,

Liu²,

Zeng³

et al. 2023

Catal. Sci. Technol.

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Section: Catalytic Hydroconversion Processes For Deconstruction Of Po...mentioning

confidence: 92%

Section: Catalytic Hydroconversion Processes For Deconstruction Of Po...mentioning

confidence: 99%

Section: Catalytic Hydroconversion Processes For Deconstruction Of Po...mentioning

confidence: 99%

See 1 more Smart Citation

Catalytic hydroconversion processes for upcycling plastic waste to fuels and chemicals

Wei¹,

Liu²,

Zeng³

et al. 2023

Catal. Sci. Technol.

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“…Second, catalysts known for low-temperature hydroconversion (mainly 200°to 300°C) generally use noble metals (Fig. 1A) (18)(19)(20)(21)(22)(23), leading to prohibitively high operating cost according to techno-economic analysis (24). High selectivity to form low-value methane due to the rapid breakage of terminal C─C bond is another issue often encountered by relatively active catalysts using noble metals, especially Ru (25,26).…”

Section: Introductionmentioning

confidence: 99%

A reusable, impurity-tolerant and noble metal–free catalyst for hydrocracking of waste polyolefins

et al. 2023

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One-step conversion of low-purity polyolefins to value-added products without pretreatments represents a great opportunity for chemical recycling of waste plastics. However, additives, contaminants, and heteroatom-linking polymers tend to be incompatible with catalysts that break down polyolefins. Here, we disclose a reusable, noble metal–free and impurity-tolerant bifunctional catalyst, MoS x -Hbeta, for hydroconversion of polyolefins into branched liquid alkanes under mild conditions. The catalyst works for a wide scope of polyolefins, including different kinds of high–molecular weight polyolefins, polyolefins mixed with various heteroatom-linking polymers, contaminated polyolefins, and postconsumer polyolefins with/without cleaning under 250°C and 20 to 30 bar H 2 in 6 to 12 hours. A 96% yield of small alkanes was successfully achieved even at a temperature as low as 180°C. These results demonstrate the great potentials of hydroconversion in practical use of waste plastics as a largely untapped carbon feedstock.

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“…Numerous catalytic and noncatalytic methodologies have recently emerged to deconstruct POs. Hydrogenolysis, − hydrocracking, − and alkane metathesis , were demonstrated to convert POs to fuel, wax, and lubricant-ranged hydrocarbons, whereas acid cracking and pyrolysis − produce a mixture of aliphatic, olefinic, and aromatic products. PO hydrogenolysis is attractive due to its mild reaction temperatures and tunable product selectivity.…”

mentioning

confidence: 99%

Structure–Property Relationships for Nickel Aluminate Catalysts in Polyethylene Hydrogenolysis with Low Methane Selectivity

Vance

Najmi

Kots

et al. 2023

JACS Au

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Earth-abundant metals have recently been demonstrated as cheap catalyst alternatives to scarce noble metals for polyethylene hydrogenolysis. However, high methane selectivities hinder industrial feasibility. Herein, we demonstrate that low-temperature ex-situ reduction (350 °C) of coprecipitated nickel aluminate catalysts yields a methane selectivity of <5% at moderate polymer deconstruction (25–45%). A reduction temperature up to 550 °C increases the methane selectivity nearly sevenfold. Catalyst characterization (XRD, XAS, 27Al MAS NMR, H2 TPR, XPS, and CO-IR) elucidates the complex process of Ni nanoparticle formation, and air-free XPS directly after reaction reveals tetrahedrally coordinated Ni2+ cations promote methane production. Metallic and the specific cationic Ni appear responsible for hydrogenolysis of internal and terminal C–C scissions, respectively. A structure-methane selectivity relationship is discovered to guide the design of Ni-based catalysts with low methane generation. It paves the way for discovering other structure–property relations in plastics hydrogenolysis. These catalysts are also effective for polypropylene hydrogenolysis.

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Structure-activity relationship in hydrogenolysis of polyolefins over Ru/support catalysts

Cited by 58 publications

References 37 publications

Catalytic hydroconversion processes for upcycling plastic waste to fuels and chemicals

Catalytic hydroconversion processes for upcycling plastic waste to fuels and chemicals

A reusable, impurity-tolerant and noble metal–free catalyst for hydrocracking of waste polyolefins

Structure–Property Relationships for Nickel Aluminate Catalysts in Polyethylene Hydrogenolysis with Low Methane Selectivity

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