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Nanostructured Nickel/Silica Catalysts for Continuous Flow Conversion of Levulinic Acid to ?-Valerolactone.

ABSTRACT: Selective transformation of levulinic acid (LA) to ?-valerolactone (GVL) using novel heterogeneous catalysts is one of the promising strategies for viable biomass processing. In this framework, we developed a continuous flow process for the selective hydrogenation of LA to GVL using several nanostructured Ni/SiO₂ catalysts. The structural, textural, acidic, and redox properties of Ni/SiO₂ catalysts, tuned by selectively varying the Ni amount from 5 to 40 wt %, were critically investigated using numerous materials characterization techniques. Electron microscopy images showed the formation of uniformly dispersed Ni nanoparticles on the SiO₂ support, up to 30% Ni loading (average particle size is 9.2 nm), followed by a drastic increase in the particles size (21.3 nm) for 40% Ni-loaded catalyst. The fine dispersion of Ni particles has elicited a synergistic metal-support interaction, especially in 30% Ni/SiO₂ catalyst, resulting in enhanced acidic and redox properties. Among the various catalysts tested, the 30% Ni/SiO₂ catalyst showed the best performance with a remarkable 98% selectivity of GVL at complete conversion of LA for 2 h reaction time. Interestingly, this catalyst showed a steady selectivity to GVL (>97%), with a 54.5% conversion of LA during 20 h time-on-stream. The best performance of 30% Ni/SiO₂ catalyst was attributed to well-balanced catalytic properties, such as ample amounts of strong acidic sites and abundant active metal sites. The obtained results show a great potential of applying earth-abundant nickel/silica catalysts for upgrading biomass platform molecules into value-added chemicals and high-energy-density fuels.

SUBMITTER: Mallesham B

PROVIDER: S-EPMC6644063 | biostudies-literature | 2018 Dec

REPOSITORIES: biostudies-literature

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Nanostructured Nickel/Silica Catalysts for Continuous Flow Conversion of Levulinic Acid to γ-Valerolactone.

Mallesham Baithy B Sudarsanam Putla P Venkata Shiva Reddy Bellala B Govinda Rao Bolla B Reddy Benjaram M BM

ACS omega 20181207 12

Selective transformation of levulinic acid (LA) to γ-valerolactone (GVL) using novel heterogeneous catalysts is one of the promising strategies for viable biomass processing. In this framework, we developed a continuous flow process for the selective hydrogenation of LA to GVL using several nanostructured Ni/SiO<sub>2</sub> catalysts. The structural, textural, acidic, and redox properties of Ni/SiO<sub>2</sub> catalysts, tuned by selectively varying the Ni amount from 5 to 40 wt %, were critical ...[more]

PMID: 31458310

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Project description:The development of reliable production routes for sustainable hydrogen (H2), which is an essential feedstock for industrial processes and energy carrier for fuel cells, is needed. It appears to be an unavoidable alternative to significantly reduce the dependence on conventional energy sources based on fossil fuels without increasing the atmospheric CO2 levels. Among the different power-to-X scenarios to access high purity H2, the electrochemical approach based on electrolysis looks to be a promising sustainable solution at both the small and large industrial scales. However, the practical realization of this important opportunity faces several challenges, including the efficient design of cost-effective catalytic materials to be used as a cathode with improved intrinsic and durable activity. In this contribution, we report the design and development of efficient nanostructured catalysts for the electrocatalytic hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in aqueous media, whereby noble metal-free elements are embedded in a matrix of a conducting polymer, polyaniline (PANI). To increase the electrical conductivity and further the electrocatalytic ability toward HER of the chemically polymerized PANI in the presence of nickel (II) salt (nitrate), the PANI-based materials have first been stabilized at a mild temperature of 250-350°C in air and then carbonized at 800-1,000°C under nitrogen gas to convert the chemical species into nitrogen, sulfur, nickel, and carbon nanostructured networks (CNNs). Different physicochemical (TGA-DSC, Raman spectroscopy, XRD, SEM, EDX, ICP, CHNS, BET, and XPS) and electrochemical (voltammetry and electrochemical impedance spectrometry) methods have been integrated to characterize the as-synthesized CNNs materials and interrogate the relationship of material-to-performance. It has been found that those synthesis conditions allow for the substantial increase of the electrocatalytic performance toward HER and OER in alkaline media in terms of the onset potential and charge transfer resistance and overpotential at the specific activity of 10 milliamps per square centimeter, thus ranking the present materials among the most efficient noble metal-free catalysts and making them possible candidates for integration in practical low-energy consumption alkaline electrolyzers.

Dataset Information

Nanostructured Nickel/Silica Catalysts for Continuous Flow Conversion of Levulinic Acid to ?-Valerolactone.

Publications

Nanostructured Nickel/Silica Catalysts for Continuous Flow Conversion of Levulinic Acid to γ-Valerolactone.

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