Enhanced activity of a bifunctional Pt/zeolite Y catalyst with an intracrystalline hierarchical pore system in the aqueous-phase hydrogenation of levulinic acid

Vu, Hue-Tong; Harth, Florian M.; Goepel, Michael; Linares, Noemi; García‐Martínez, Javier; Gläser, Roger

doi:10.1016/j.cej.2021.132763

Cited by 25 publications

(8 citation statements)

References 54 publications

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“…Therefore, the non-local density functional theory (NLDFT) was employed to determine the pore structure. 41 It is revealed that micropores dominate in all the tested samples as shown in Table 3 . Regardless of Al to Si ratios, a similar specific total pore volume (0.20–0.22 cm 3 g −1 ) and a pore structure comprising 70% of micropores and 30% of mesopores are observed in the N 2 sorption results.…”

Section: Resultsmentioning

confidence: 83%

Insight into the interdependence of Ni and Al in bifunctional Ni/ZSM-5 catalysts at the nanoscale

Arčon

Souza

et al. 2022

Nanoscale Adv.

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Section: Resultsmentioning

confidence: 83%

Insight into the interdependence of Ni and Al in bifunctional Ni/ZSM-5 catalysts at the nanoscale

Arčon

Souza

et al. 2022

Nanoscale Adv.

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“…To further confirm the Pt content, inductive coupled plasma–optical emission spectroscopy (ICP–OES) was applied using Agilent Technologies 700 series. The samples were digested with concentrated HF/HCl/HNO 3 with a volume ratio of 2:3:3 and saturated with H 3 BO 4 analysis for balancing out the excessive HF . The basicity of the catalysts was measured by temperature-programmed desorption of carbon dioxide (CO 2 -TPD) recorded on a BELCAT II chemisorption analyzer.…”

Section: Methodsmentioning

confidence: 99%

“…The samples were digested with concentrated HF/HCl/HNO 3 with a volume ratio of 2:3:3 and saturated with H 3 BO 4 analysis for balancing out the excessive HF. 62 The basicity of the catalysts was measured by temperature-programmed desorption of carbon dioxide (CO 2 -TPD) recorded on a BELCAT II chemisorption analyzer. Before analysis, the catalyst was outgassed under He gas at 300 °C for 1 h. Afterward, the sample was saturated with CO 2 at 100 °C for 30 min and then purged with He to remove the physically adsorbed CO 2 for 30 min.…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

Pt Nanoparticles on ZSM-5 Nanoparticles for Base-Free Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid

Salakhum

Prasertsab

Pornsetmetakul

et al. 2021

ACS Appl. Nano Mater.

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5-Hydroxymethylfurfural (HMF) is considered as a valuable platform chemical derived from abundant sugars in a plant-based biomass. One of the most precious chemicals, which can be derived from HMF, is 2,5-furandicarboxylic acid (FDCA), which is a renewable substituent for petroleum-based terephthalic acid. Herein, the selective oxidation of HMF to FDCA and its derivatives has been accomplished using highly dispersed Pt nanoparticles supported on alkaline-exchanged hierarchical ZSM-5 nanoparticles under mild conditions (110 °C and 2.0 MPa of air) in a base-free aqueous-phase system. Interestingly, a high HMF conversion (100%) with 80% of FDCA selectivity was achieved. The synergetic effect of highly dispersed Pt nanoparticles and an alkaline-exchanged framework plays a key role, wherein they act as active oxidative sites for this multi-oxidation reaction. These findings open up prospects for the development of zeolite-based catalysts for the conversion of HMF to high value-added FDCA and its derivatives in a base-free aqueous system.

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“…In this regard, ZrO 2 -based catalysts were the first to facilitate the conversion of LA and LE to GVL with secondary alcohols (e.g., 2-propanol and 2-butanol) as a hydrogen source. Zr hydroxide ZrO(OH) 2 · x H 2 O and mesoporous zeolites with large surface areas , were also found effective for GVL production. An additional advantage of using zeolites is that the ratio of Lewis to Brønsted acid sites can be mediated, thus improving GVL selectivity. , …”

Section: Introductionmentioning

confidence: 99%

Multisite Porphyrinic Metal–Organic Frameworks for Biomass Valorization: Computational Design and Mechanistic Investigation

Krishnan

Yang

Jiang

2023

ACS Sustainable Chem. Eng.

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Renewable chemicals and fuels have received significant attention for sustainable economic development. Our aim in this work is to investigate a porphyrinic metal–organic framework (MOF), namely, MOF-525 for the transfer hydrogenation of methyl levulinate (ML) to γ-valerolactone (GVL) through density functional theory calculations. We computationally design five multisite defect-engineered MOF-525(M) (M = CrIII, FeIII, RuIII, RhIII, and IrIII) and examine their catalytic performance for the transformation of ML to methyl valerate (MV) via catalytic transfer hydrogenation (CTH), subsequently for the cyclization of MV to GVL by anchoring a SO3H group as a Brønsted acid site on the metallated linker M-TPP-Cl. The CTH involves three pathways (two concerted and one stepwise) on the defective Zr node and two pathways (one stepwise and one concerted) on the metallated linker, respectively. It is revealed that a stepwise Meerwein–Ponndorf–Verley pathway is energetically preferred on the defective Zr node. A similar stepwise pathway on Ru-TPP-Cl is also found to be favorable, while a concerted pathway is more favorable on Rh-TPP-Cl and Ir-TPP-Cl. The rate-determining activation barriers on M-TPP-Cl are rationalized by geometry analysis, second-order perturbation theory analysis, and the noncovalent interactions. Among the five metallated MOF-525(M), Ru, Rh, and Ir are predicted to be active for the transformation of ML to MV. However, the defective Zr-SBU is found to have a lower activation energy barrier compared to M-TPP-Cl, suggesting its dominant role in CTH. In addition, the Brønsted acid-catalyzed cyclization appears to be rate-determining on the defective Zr node, Rh-TPP-Cl, and Ir-TPP-Cl. This study suggests that MOF-525 might be potentially used as a multisite catalyst platform for the conversion of ML to GVL and would assist in the future rational design of new MOFs for biomass valorization.

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Enhanced activity of a bifunctional Pt/zeolite Y catalyst with an intracrystalline hierarchical pore system in the aqueous-phase hydrogenation of levulinic acid

Cited by 25 publications

References 54 publications

Insight into the interdependence of Ni and Al in bifunctional Ni/ZSM-5 catalysts at the nanoscale

Insight into the interdependence of Ni and Al in bifunctional Ni/ZSM-5 catalysts at the nanoscale

Pt Nanoparticles on ZSM-5 Nanoparticles for Base-Free Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid

Multisite Porphyrinic Metal–Organic Frameworks for Biomass Valorization: Computational Design and Mechanistic Investigation

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