Synthesis of Mo and Ru solid-solution alloy NPs and their hydrogen evolution reaction activity

Okazoe, Shinya; Kusada, Kohei; Wu, Dongshuang; Yamamoto, Tomokazu; Toriyama, Takaaki; Matsumura, Shuichi; Kawaguchi, Shogo; Kubota, Yoshiki; Kitagawa, Hiroshi

doi:10.1039/d0cc05958g

Cited by 29 publications

(23 citation statements)

References 30 publications

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“…The calculated lattice constants of Mo 0.2 Ru 0.8 NPs ( a =2.7706 Å, c =4.3289 Å for a hcp structure, a =3.8530 Å for a fcc structure) were slightly larger than those of Ru NPs ( a =2.7109 Å, c =4.2879 Å for a hcp structure, a =3.8202 Å for a fcc structure), which indicates alloying Ru with Mo which has a larger atomic radius. These results support the formation of a solid‐solution alloy with lattice parameters that are larger than those of Ru, as previously reported [11] …”

Section: Methodssupporting

confidence: 92%

“…Ru NPs and MoRu solid‐solution alloy NPs were synthesized by thermal decomposition [11] and denoted as Ru and Mo 0.2 Ru 0.8 (see the Supporting Information, SI). The exact atomic ratio of Mo and Ru in MoRu solid‐solution alloy NPs was calculated to be 0.19 : 0.81 by X‐ray fluorescence (XRF) spectroscopy.…”

Section: Methodsmentioning

confidence: 99%

“…These results support the formation of a solid-solution alloy with lattice parameters that are larger than those of Ru, as previously reported. [11] These NPs were applied in the catalytic hydrogenation of unsaturated hydrocarbons (1-octene and 1-octyne) (Scheme 1). Hydrogenation tests were performed with 1 mol% NPs toward the substrates in 2.4 mL of tetrahydrofuran (THF).…”

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confidence: 99%

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Enhanced Hydrogenation Catalytic Activity of Ruthenium Nanoparticles by Solid‐Solution Alloying with Molybdenum

et al. 2021

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We report the hydrogenation catalytic activity application of molybdenum–ruthenium (MoRu) solid‐solution alloy nanoparticles (NPs) as catalysts for the hydrogenation of 1‐octene and 1‐octyne. The solid‐solution structure of MoRu NPs was confirmed through scanning transmission electron microscopy (STEM) coupled with energy‐dispersive X‐ray spectroscopy (EDX), and powder X‐ray diffraction (PXRD) measurement. The hydrogenation catalytic activity of these NPs toward 1‐octyne and 1‐octene in tetrahydrofuran (THF) was tested. The hydrogenation catalytic activity of Ru was enhanced by alloying with Mo at the atomic level. An electronic modification of Ru by a charge transfer from Mo to Ru, which could induce the change in the adsorption energy of reactants resulting in enhanced catalytic activity, was observed by X‐ray photoelectron spectroscopy.

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Section: Methodssupporting

confidence: 92%

Section: Methodsmentioning

confidence: 99%

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confidence: 99%

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Enhanced Hydrogenation Catalytic Activity of Ruthenium Nanoparticles by Solid‐Solution Alloying with Molybdenum

et al. 2021

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“…c, Representative Ru hemispherical particle partially covered by an overlayer. d, High magnification image indicating a lattice spacing of 2.38 Å, consistent with Ru(100), and a lattice spacing of ∼3.6 Å of the overlayer, consistent with monoclinic WO 3 . , e and f, DF-STEM images of Ru-15WZr indicating a uniform distribution of the ∼1 nm WO x clusters. g, STEM-EDS elemental mapping of the Ru-15WZr catalyst.…”

Section: Resultsmentioning

confidence: 99%

Polyethylene Hydrogenolysis at Mild Conditions over Ruthenium on Tungstated Zirconia

Wang

Xie

Kots

et al. 2021

JACS Au

158

146

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Plastics waste has become a major environmental threat, with polyethylene being one of the most produced and hardest to recycle plastics. Hydrogenolysis is potentially the most viable catalytic technology for recycling. Ruthenium (Ru) is one of the most active hydrogenolysis catalysts but yields too much methane. Here we introduce ruthenium supported on tungstated zirconia (Ru-WZr) for hydrogenolysis of low-density polyethylene (LDPE). We show that the Ru-WZr catalysts suppress methane formation and produce a product distribution in the diesel and wax/lubricant base-oil range unattainable by Ru-Zr and other Ru-supported catalysts. Importantly, the enhanced performance is showcased for real-world, single-use LDPE consumables. Reactivity studies combined with characterization and density functional theory calculations reveal that highly dispersed (WO x ) n clusters store H as surface hydroxyls by spillover. We correlate this hydrogen storage mechanism with hydrogenation and desorption of long alkyl intermediates that would otherwise undergo further C–C scission to produce methane.

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“…[1] Electrochemical water splitting is a highly promising technology for producing highly pure hydrogen through the cathode hydrogen evolution reaction (HER). [2,3] Therefore, exploiting efficient cathodic active electrocatalyst is significantly critical to accelerate the HER process that has sluggish kinetics and large overpotentials. [4][5][6] Although the platinum (Pt)-based materials possess the fascinating catalytic activity for HER, high price and low reserves are still obstacles to their large-scale application.…”

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confidence: 99%

Rational Construction of Ruthenium‐Cobalt Oxides Heterostructure in ZIFs‐Derived Double‐Shelled Hollow Polyhedrons for Efficient Hydrogen Evolution Reaction

Fan

Tian

Yan

et al. 2021

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Transition metal oxides (TMOs) and their heterostructure hybrids have emerged as promising candidates for hydrogen evolution reaction (HER) electrocatalysts based on the recent technological breakthroughs and significant advances. Herein, Ru‐Co oxides/Co3O4 double‐shelled hollow polyhedrons (RCO/Co3O4‐350 DSHPs) with Ru‐Co oxides as an outer shell and Co3O4 as an inner shell by pyrolysis of core‐shelled structured RuCo(OH)x@zeolitic‐imidazolate‐framework‐67 derivate at 350 °C are constructed. The unique double‐shelled hollow structure provides the large active surface area with rich exposure spaces for the penetration/diffusion of active species and the heterogeneous interface in Ru‐Co oxides benefits the electron transfer, simultaneously accelerating the surface electrochemical reactions during HER process. The theory computation further indicates that the existence of heterointerface in RCO/Co3O4‐350 DSHPs optimize the electronic configuration and further weaken the energy barrier in the HER process, promoting the catalytic activity. As a result, the obtained RCO/Co3O4‐350 DSHPs exhibit outstanding HER performance with a low overpotential of 21 mV at 10 mA cm−2, small Tafel slope of 67 mV dec−1, and robust stability in 1.0 m KOH. This strategy opens new avenues for designing TMOs with the special structure in electrochemical applications.

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Synthesis of Mo and Ru solid-solution alloy NPs and their hydrogen evolution reaction activity

Abstract: We report the synthesis of MoRu solid-solution alloy nanoparticles using carbonyl complexes as a precursor through a thermal decomposition, and their catalytic activity for hydrogen evolution reaction.

Cited by 29 publications

References 30 publications

Enhanced Hydrogenation Catalytic Activity of Ruthenium Nanoparticles by Solid‐Solution Alloying with Molybdenum

Enhanced Hydrogenation Catalytic Activity of Ruthenium Nanoparticles by Solid‐Solution Alloying with Molybdenum

Polyethylene Hydrogenolysis at Mild Conditions over Ruthenium on Tungstated Zirconia

Rational Construction of Ruthenium‐Cobalt Oxides Heterostructure in ZIFs‐Derived Double‐Shelled Hollow Polyhedrons for Efficient Hydrogen Evolution Reaction

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