Highly dispersed supported ruthenium oxide as an aerobic catalyst for acetic acid synthesis

Laursen, Anders B.; Gorbanev, Yury; Cavalca, Filippo; Kleiman-Schwarsctein, Alan; Kegnæs, Søren; Riisager, Anders; Chorkendorff, Ib; Dahl, Søren

doi:10.1016/j.apcata.2012.05.025

Cited by 14 publications

(9 citation statements)

References 35 publications

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“…The Ru peaks are located between 461.2 eV (Ru 0 ) and 463.3 eV (RuO 2 ), indicating the oxidation state of Ru δ+ (0 < δ < 4). Compared to those of Ru/pBN-0.58%F and -1.13%F, the Ru peaks of Ru/pBN-0.56%R and -1.13%R show high binding energies, closer to the 463.3 eV of RuO 2 (Figures S13 and S14), which indicates the higher Ru valence state in Ru/pBN- x R than that in Ru/pBN- x F samples. , The high Ru valence state in Ru/pBN- x R may be attributed to the O-enriched pBN support due to the high electron-withdrawing property of O (Figure S10). , X-ray absorption near-edge structure (XANES) spectra show that the Ru K edge of Ru/pBN-0.58%F yields a white line between Ru foil and RuO 2 (Figure d), indicating that Ru has the positive charge of Ru δ+ (0 < δ < 4) resulting from Ru–O/N/B bonds .…”

Section: Resultsmentioning

confidence: 99%

Atomic Ru Immobilized on Porous h-BN through Simple Vacuum Filtration for Highly Active and Selective CO₂ Methanation

Fan

Jiménez

Shirodkar³

et al. 2019

ACS Catal.

101

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As CO 2 emissions are sharply increasing, processes for converting CO 2 into value-added products are becoming more desirable. Ruthenium-based catalysts are the most active for CO 2 methanation; however, their substantially higher cost relative to transition metals makes them prohibitive for industrial application. In this study, we demonstrate porous hexagonal boron nitride (pBN) supports (an ideal support material for thermocatalysts due to the high thermal stability and conductivity) to improve the utilization of Ru and simultaneously enhance the catalytic activity and selectivity for CO 2 methanation. A simple vacuum filtration process is proposed that allows the Ru precursor to quickly locate the defects of pBN, where atomic Ru can be restricted onto the defects via B, N coordination through an annealing treatment. The B and N coordinations reduce the valence state of atomic Ru. The as-prepared catalyst with low Ru loading (0.58 wt %) exhibits CH 4 selectivity up to 93.5%, catalytic stability after 110 h, and a higher reaction rate [1.86 mmol CO 2 /(g cat s)] at 350 °C and 1.0 MPa compared to other nanoparticle catalysts. Both atomic-scale size and low valence state of atomic Ru supported on pBN are responsible for the improvement of CH 4 production rate as confirmed by density functional theory simulation.

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Section: Resultsmentioning

confidence: 99%

Atomic Ru Immobilized on Porous h-BN through Simple Vacuum Filtration for Highly Active and Selective CO₂ Methanation

Fan

Jiménez

Shirodkar³

et al. 2019

ACS Catal.

101

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“…Additionally, catalytic upgrading of biomass and derived compounds have been reported over various supported ruthenium oxide catalysts. 16,[36][37][38][39][40][41][42] The many applications of ruthenium in catalysis has rendered it a very wellstudied metal in both homogeneous and heterogeneous systems. [43][44][45][46][47][48][49][50][51][52][53][54] More recently, Mizuno and Yamaguchi reported high activity of supported ruthenium hydroxide catalysts (Ru(OH)x/support) in liquid-phase oxidations of alcohols, aldehydes and amines.…”

Section: Introductionmentioning

confidence: 99%

Selective formation of formic acid from biomass-derived glycolaldehyde with supported ruthenium hydroxide catalysts

Modvig

Riisager

2019

Catal. Sci. Technol.

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“…S3 †), corresponding to the metallic Ru, Ru/RuO y , RuCl 3 , RuO 2 and RuO x species, respectively. [34][35][36][37] The relative content and binding energy of all the ve Ru species are listed in Table 2. This indicates that the dominant species of Ru-in-CNT are RuO 2 (46.6%) followed by Ru/RuO y (24.4%), RuO x (14.5%), RuCl 3 (10.9%) and metallic Ru (3.6%), while the major species of Ruout-CNT include metallic Ru (28.1%), RuO 2 (25.9%) and RuCl 3 (24.5%).…”

Section: Resultsmentioning

confidence: 99%

Non-mercury catalytic acetylene hydrochlorination over Ru catalysts enhanced by carbon nanotubes

Zhang

et al. 2015

RSC Adv.

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Highlights• Ru catalysts deposited inside the channels of CNTs show higher catalytic activity.• Ru-in-CNT catalyst exhibited the acetylene conversion of 95.0 % at 170 °C and 10 h.• CNTs with the inner diameter of 3-7 nm can functionalize as an efficient support.Abstract 1 Ru-based catalysts with different deposition sites were prepared using multiwalled carbon 2 nanotubes as the support and RuCl 3 as the precursor, in order to study the effects of multiwalled 3 carbon nanotubes on the catalytic performance of Ru catalysts for acetylene hydrochlorination. It 4 is suggested that Ru catalysts deposited inside the CNTs channels exhibit the optimal catalytic 5 activity, with the acetylene conversion of 95.0 % and the selectivity to VCM of 99.9 % after 10 h 6 on stream under the conditions of 170 °C and GHSV (C 2 H 2 ) of 90 h -1 . In combination with 7 characterizations of BET, TEM, XRD, TPR, TPD and XPS, it is illustrated that the CNTs with 8 the inner diameter about 3-7 nm can functionalize as an efficient support with unique electron 9 property to enhance the catalytic performance of Ru-based catalysts for acetylene 10 hydrochlorination.11

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Highly dispersed supported ruthenium oxide as an aerobic catalyst for acetic acid synthesis

Cited by 14 publications

References 35 publications

Atomic Ru Immobilized on Porous h-BN through Simple Vacuum Filtration for Highly Active and Selective CO₂ Methanation

Atomic Ru Immobilized on Porous h-BN through Simple Vacuum Filtration for Highly Active and Selective CO₂ Methanation

Selective formation of formic acid from biomass-derived glycolaldehyde with supported ruthenium hydroxide catalysts

Non-mercury catalytic acetylene hydrochlorination over Ru catalysts enhanced by carbon nanotubes

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Highly dispersed supported ruthenium oxide as an aerobic catalyst for acetic acid synthesis

Cited by 14 publications

References 35 publications

Atomic Ru Immobilized on Porous h-BN through Simple Vacuum Filtration for Highly Active and Selective CO2 Methanation

Atomic Ru Immobilized on Porous h-BN through Simple Vacuum Filtration for Highly Active and Selective CO2 Methanation

Selective formation of formic acid from biomass-derived glycolaldehyde with supported ruthenium hydroxide catalysts

Non-mercury catalytic acetylene hydrochlorination over Ru catalysts enhanced by carbon nanotubes

Contact Info

Product

Resources

About

Atomic Ru Immobilized on Porous h-BN through Simple Vacuum Filtration for Highly Active and Selective CO₂ Methanation

Atomic Ru Immobilized on Porous h-BN through Simple Vacuum Filtration for Highly Active and Selective CO₂ Methanation