Effect of carbon supports on RhRe bifunctional catalysts for selective hydrogenolysis of tetrahydropyran-2-methanol

Karanjkar, Pranav U.; Burt, Samuel P.; Chen, Xiaoli; Barnett, Kevin J.; Ball, Madelyn R.; Kumbhalkar, Mrunmayi D.; Wang, Xiaohong; Miller, James B.; Hermans, Ive; Dumesic, James A.; Huber, George W.

doi:10.1039/c6cy01763k

Cited by 28 publications

(13 citation statements)

References 36 publications

(63 reference statements)

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“…These are attributed to B−O−H deformations, [49,51–54] B−O stretching of BO 3 units, [53–55] and C=C stretching from the support, respectively [47] . On non‐borated OAC, the features at 1756 and 1580 cm −1 are assigned to C=O and conjugated aromatic C=C functional groups, respectively [47,56] . It is important to note that C=O peak at 1756 cm −1 is absent in B/OAC (fresh and spent), suggesting a high fraction of C=O sites on the surface of the carbon support are consumed by boron during impregnation of H 3 BO 3 (Figure 1).…”

Section: Resultsmentioning

confidence: 99%

“…Deconvolution of the broad OAC peak at 1240 cm −1 results in 3 species at 1115, 1238, and 1398 cm −1 (Figure 4b). These are attributed to oxygen functionalities of either C−O‐C, [56] O−H bending or C−O stretching, [47] and carboxylic acid −O−H bending [57] . Much of this broad peak appears to be consumed following boron impregnation as evidenced by the absence of such a peak in the fresh and spent B/OAC spectra, corroborating the observation that boron consumes C=O/C−O species on the surface of the carbon support.…”

Section: Resultsmentioning

confidence: 99%

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Highly Selective Carbon‐Supported Boron for Oxidative Dehydrogenation of Propane

et al. 2021

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Bulk boron materials, such as hexagonal boron nitride (h‐BN), are highly selective catalysts for the oxidative dehydrogenation of propane (ODHP). Previous attempts to improve the productivity of these systems involved the immobilization of boron on silica and resulted in less selective catalysts. Here, we report that acid‐treated, activated carbon‐supported boron prepared via incipient wetness impregnation with boric acid (B/OAC) exhibits equal propylene selectivity and improved productivity (kgpropylene kgcat−1 hr−1) as compared to h‐BN. Characterization of the fresh and spent catalysts with infrared, Raman, X‐ray photoelectron, and solid‐state NMR spectroscopies reveals the presence of oxidized/hydrolyzed boron that is clustered on the surface of the support.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Highly Selective Carbon‐Supported Boron for Oxidative Dehydrogenation of Propane

et al. 2021

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“…17 Karanjkar et al reported an enhanced hydrogenolysis of cyclic ethers, such as tetrahydropyran-2-methanol, over a ReO x -promoted Rh/C catalyst. 18 Regarding phenol derivatives, Lamb et al reported Pd-Re bimetallic synergy for the HDO of guaiacol to cyclohexane. 19 The enhanced HDO activity of these bimetallic catalysts is generally understood to follow a bifunctional mechanism, in which the noble metals, such as Pd and Rh, provide the hydrogenation function, and Re (or ReO x ) promotes the deoxygenation activity.…”

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confidence: 99%

Bimetallic Ni‐Re catalysts for the efficient hydrodeoxygenation of biomass‐derived phenols

Park

Kim

et al. 2021

Int J Energy Res

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The development of non-noble metal-based catalysts for the hydrodeoxygenation (HDO) upgrading of biomass pyrolysis oils is crucial for realizing the cost-effective biofuel production. In this paper, we report on the enhanced HDO activity of the rhenium-promoted nickel catalysts (Ni-Re) for the HDO of a pyrolysis oil model compound, guaiacol. The catalyst screening studies revealed that the Ni-Re displayed a considerably higher HDO activity than other monometallic (Ni, Re, Cu, Co) and bimetallic catalysts (Cu-Re, Co-Re), highlighting its unique catalytic property. In order to optimize the catalytic activity and reveal the structure-activity relationship of the Ni-Re catalysts, the effects of the Ni/Re ratio and type of support (SiO 2 , TiO 2 , and ZrO 2 ) on the catalyst structure and HDO activity were investigated in detail. The results showed that the addition of rhenium to nickel altered both geometric and electronic structures of nickel significantly. The Ni-Re/SiO 2 catalyst with a Ni/Re ratio of 0.315 achieved~95% yield of the desired deoxygenation product, cyclohexane, at 523 K and 30 bar-H 2 after 5 hours. Novelty StatementThe upgrading of biomass pyrolysis oils to hydrocarbon fuels oftentimes requires the use of noble metal catalysts and harsh reaction conditions (e.g., high H 2 pressure), all of which greatly increase the process cost. In this work, a highly active and nonprecious metal-based catalyst, bimetallic Ni-Re/SiO 2 , is developed for the cost-effective upgrading of biomass-derived phenols to deoxygenated hydrocarbon fuels at low temperature and low pressure.

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“…The electrocatalysts without Nb displayed a higher contact angle (Figure ), indicating higher hydrophobicity than electrocatalysts containing Nb. The hydrophilicity of an electrocatalyst plays an important role in heterogeneous catalysis, due to the bifunctional effect of weakly H 2 O adsorption and dissociating to OH − +H + ions . Thus, Nb addition to the electrocatalysts favors the bifunctional mechanism.…”

Section: Resultsmentioning

confidence: 99%

“…The hydrophilicity of an electrocatalyst plays an important role in heterogeneous catalysis, due to the bifunctional effect of weakly H 2 O adsorption and dissociating to OH À + H + ions. [14,32] Thus, Nb addition to the electrocatalysts favors the bifunctional mechanism.…”

Section: Physicochemical Characterizationmentioning

confidence: 99%

Niobium Enhances Electrocatalytic Pd Activity in Alkaline Direct Glycerol Fuel Cells

et al. 2019

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Pd x Nb y /C binary electrocatalysts supported on Printex 6 L carbon black were prepared by using an adapted chemical reduction method with sodium borohydride. The electrocatalysts were characterized by using SEM, TEM, XRD, EDS, ICP-MS, water contact angle and Raman spectroscopy. The best performance for the alkaline direct glycerol fuel cell (ADGFC) was obtained by using Pd 1 Nb 1 /C, which yielded a maximum power density of 27 mW cm À 2 at 70°C. Residues of products formed from the glycerol oxidation were analyzed by using FT-Raman and high-performance liquid chromatography (HPLC).The Pd 1 Nb 1 /C electrocatalyst exhibited a more negative onset potential for the CO oxidation reaction and a higher conversion rate of glycerol to carbonate. We suggest that the higher hydrophilicity, higher degree of disorder, and bifunctional effects enhanced the electrocatalytic activity of Pd, as Nb facilitated the oxidation of adsorbed CO in Pd and increased the transfer rate of electron from Pd to carbon black support Therefore, Nb is a promising co-catalyst for Pd-based electrocatalysts for ADGFCs.

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Effect of carbon supports on RhRe bifunctional catalysts for selective hydrogenolysis of tetrahydropyran-2-methanol

Abstract: Orders-of-magnitude differences in hydrogenolysis activity were observed between RhRe/C catalysts with different carbon supports, which is due to the types of bimetallic particles that are formed on the different carbon supports.

Cited by 28 publications

References 36 publications

Highly Selective Carbon‐Supported Boron for Oxidative Dehydrogenation of Propane

Highly Selective Carbon‐Supported Boron for Oxidative Dehydrogenation of Propane

Bimetallic Ni‐Re catalysts for the efficient hydrodeoxygenation of biomass‐derived phenols

Niobium Enhances Electrocatalytic Pd Activity in Alkaline Direct Glycerol Fuel Cells

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