Role of Brønsted and Lewis acid sites on Ni/TiO2 catalyst for vapour phase hydrogenation of levulinic acid: Kinetic and mechanistic study

Kumar, Velisoju Vijay; Gutta, Naresh; Sudhakar, M.; Tardio, James; Bhargava, Suresh K.; Venugopal, A.

doi:10.1016/j.apcata.2015.07.031

Cited by 122 publications

(78 citation statements)

References 34 publications

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“…Balla et al . and Kumar and co‐workers showed that catalytic activity in the gas phase transformation of LA → AGL is dependent on the concentration and type of acid sites.…”

Section: Resultsmentioning

confidence: 99%

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Continuous gas phase catalytic transformation of levulinic acid to γ‐valerolactone over supported Au catalysts

Mustafin

Cárdenas‐Lizana

Keane

2017

J of Chemical Tech & Biotech

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BACKGROUND: -Valerolactone (GVL) is a high value chemical obtained from hydrogenation of bio-derived levulinic acid (LA). Work to date has focused on batch pressurised catalytic systems where high GVL yield is challenging. In this work, the role of support redox and acidity properties is examined in the continuous gas phase hydrogenation of aqueous LA at ambient pressure over gold on Al 2 O 3 , CeO 2 and TiO 2 ; Pd/Al 2 O 3 served as a benchmark in catalyst tests. RESULTS: 100% GVL yield was achieved under stoichiometric conditions (inlet H2 /LA = 1) over supported Au (mean size = 3.0-4.3 nm). Greater catalytic activity was recorded for Au on reducible TiO 2 and CeO 2 . Under the same reaction conditions, Pd/Al 2 O 3 delivered higher LA consumption rates but promoted formation of pentanoic acid. CONCLUSIONS: GVL formation proceeds via 4-hydroxypentanoic as reactive intermediate. Surface oxygen vacancies (confirmed by O 2 titration) formed during temperature programmed reduction of reducible oxides activate LA for reaction. Greater GVL productivity (with full hydrogen utilisation) is demonstrated in this work relative to state-of-the art supported Pd and Ru catalysts. EXPERIMENTAL Catalyst preparation and activationThe oxide carriers ( -Al 2 O 3 (Puralox, Condea Vista Co.), CeO 2 (Grace Davison) and TiO 2 (P25, Degussa)) were used as received. Supported (1.0-3.0% wt.) Au catalysts were prepared by deposition-precipitation. Urea (100-fold excess, Riedel-de Haën, 99%), used as basification agent, was added to an aqueous solution of HAuCl 4 (4 × 10 −5 -5 × 10 −3 M; 20-50 cm 3 , Sigma-Aldrich,99%) containing the support (5-30 g). The wileyonlinelibrary.com/jctb

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“…Balla et al . and Kumar and co‐workers showed that catalytic activity in the gas phase transformation of LA → AGL is dependent on the concentration and type of acid sites.…”

Section: Resultsmentioning

confidence: 99%

“…) or further conversion of GVL (step (V)). Kumar et al . has shown by combined pyridine adsorption/DRIFTS analysis and kinetic measurements that acid sites promote GVL ring opening to pentanoic acid.…”

Section: Resultsmentioning

confidence: 99%

Continuous gas phase catalytic transformation of levulinic acid to γ‐valerolactone over supported Au catalysts

Mustafin

Cárdenas‐Lizana

Keane

2017

J of Chemical Tech & Biotech

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“…Besides variations in support phase composition, many different synthetic procedures for titania-supported Ru catalyst preparation have been reported varying in the choice of, e.g., metal precursor, impregnation method and activation procedure (Table 1), which all may affect catalyst performance. Wet impregnation is most commonly used method for the synthesis of these Ru/TiO 2 catalysts [19,20,25,29], using Ru precursors such as RuCl 3 , Ru(NO)(NO 3 ) 3 , Ru(acac) 3 , Ru (NH 3 ) 6 Cl 3 or Ru 3 (CO) 12 [19,20,25,[29][30][31][32][33][34][35]. Limited information is available on the effects of these synthesis parameters on LA hydrogenation activity for Ru/TiO 2 catalysts.…”

Section: Introductionmentioning

confidence: 99%

Hydrogenation of levulinic acid to γ-valerolactone over anatase-supported Ru catalysts: Effect of catalyst synthesis protocols on activity

Piskun

Ftouni

Tang

et al. 2018

Applied Catalysis A: General

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“…[47] The catalytic performance of widely used TiO 2 supported metal catalysts with different metals including Ni, Pt, Pd and Ru was tested. [38] The highest GVL selectivity of 87.6% would be obtained over Ni/TiO 2 (Table 1, entry 9), which could be assigned to the higher metal dispersion of Ni on the TiO 2 . Effects of Lewis and Brønsted acid sites on the product generation were inspected, Ni/TiO 2 with a 20 wt % Ni loading, which provided more Lewis sites than the 5 wt % Ni/TiO 2 , could achieve a relatively optimal performance with a 99.9% LA conversion and a 99.1% GVL selectivity at 270°C ( Table 1, entry 11).…”

Section: Metallic Oxidesmentioning

confidence: 97%

“…[66] Although Brønsted acidity can promote the lactonization process to generate GVL to a certain extent, an excessive Brønsted acidity is not required for obtaining a higher GVL yield. [38,64] A further ring opening of GVL and hydrocarbons would occur with the assistance of a strong Brønsted acidity, thus greatly reducing the GVL selectivity. [90] Complete LA conversions would be given at 200°C with an 8 bar H 2 pressure for 1 h over both the Pt/SiO 2 as well as the Pt/HMFI.…”

Section: Acid-catalyzed Processmentioning

confidence: 99%

Effects of Solid Acid Supports on the Bifunctional Catalysis of Levulinic Acid to γ‐Valerolactone: Catalytic Activity and Stability

Lü

Bai

et al. 2020

Chemistry An Asian Journal

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Heterogeneous transformation of levulinic acid (LA) to γ-valerolactone (GVL) is regarded as a critical process of the lignocellulose-based biorefinery system. Substantial progress on the catalytic conversion of LA to GVL has been continuously achieved recently. However, the traditional research paradigm typically emphasizes the metal-catalyzed hydrogenation step, but lacks profound insights into the potential impacts of catalyst supports. Herein, an overview of the bifunctional catalytic system classified by representative solid acid supports for LA conversion to GVL is presented, and effects of critical factors on metal-and acid-catalyzed processes are discussed. Particularly, impacts of key issues on catalytic stability are thoroughly summarized and analyzed. Challenges and suggestions are also proposed from the perspective of increases in both catalytic activity and stability. This review potentially contributes to the rational design of high-efficiency catalysts used in the biomass valorization for renewable energy production.

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Role of Brønsted and Lewis acid sites on Ni/TiO2 catalyst for vapour phase hydrogenation of levulinic acid: Kinetic and mechanistic study

Cited by 122 publications

References 34 publications

Continuous gas phase catalytic transformation of levulinic acid to γ‐valerolactone over supported Au catalysts

Continuous gas phase catalytic transformation of levulinic acid to γ‐valerolactone over supported Au catalysts

Hydrogenation of levulinic acid to γ-valerolactone over anatase-supported Ru catalysts: Effect of catalyst synthesis protocols on activity

Effects of Solid Acid Supports on the Bifunctional Catalysis of Levulinic Acid to γ‐Valerolactone: Catalytic Activity and Stability

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