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Papers by Carlo Lucarelli

Research paper thumbnail of Steam reforming of clean biogas over Rh and Ru open-cell metallic foam structured catalysts

Research paper thumbnail of Biogas to Syngas through the Combined Steam/Dry Reforming Process: An Environmental Impact Assessment

Research paper thumbnail of Effect of exchange procedure and crystal size on high silica MFI zeolite as catalyst for vapor phase Beckmann rearrangement

Studies in Surface Science and Catalysis

ABSTRACT Caprolactam is the starting monomer for the production of Nylon-6 fibers and resins. The... more ABSTRACT Caprolactam is the starting monomer for the production of Nylon-6 fibers and resins. The current caprolactam manufacturing process is energy intensive and generates considerable wastes (ammonium sulphate). For this reason, alternative paths for the production of caprolactam providing few-step cost effective production and environmentally friendly process are required. In year 2000 Sumitomo Inc. announced the build-up of a demonstration plant for the production of caprolactam.. This process allows an ammonium sulphate-free caprolactam manufacture and will result in an industrial plant by the end of year 2003. In a recent paper Ichihashi et al. [1]claimed long-time catalytic tests with a high silica MFI zeolite which is rather active and selective towards caprolactam production. In this paper we report a study on the effect of catalyst activation method and acid sites distribution on caprolactam selectivity of high silica MFI zeolites of different crystal size. We found that catalysts activation by a NH4NO3 alkaline solution and calcinations at 450°C promotes structural rearrangement of silicalite-1 unit cell and catalytic performances remarkably higher than other silicalite-1 activated by other methods. In addition we show the direct correlation between caprolactam selectivity and H-bonded (nests of silanols and vicinal silanols) distribution.

Research paper thumbnail of Urea and Polyurea Production: An Innovative Solvent- and Catalyst-Free Approach through Catechol Carbonate

ACS Sustainable Chemistry & Engineering

Research paper thumbnail of The competition between dehydrogenation and dehydration reactions for primary and secondary alcohols over gallia: unravelling the effects of molecular and electronic structure via a two-pronged theoretical/experimental approach

Catalysis Science & Technology

The relative dehydrogenation/dehydration reactivity imparted by nanostructured gallium(iii) oxide... more The relative dehydrogenation/dehydration reactivity imparted by nanostructured gallium(iii) oxide on alcohols was investigated via electronic structure calculations, reactivity tests and DRIFT-IR spectroscopy.

Research paper thumbnail of Tandem Hydrogenation/Hydrogenolysis of Furfural to 2-Methylfuran over a Fe/Mg/O Catalyst: Structure–Activity Relationship

Catalysts

The hydrodeoxygenation of furfural (FU) was investigated over Fe-containing MgO catalysts, on a c... more The hydrodeoxygenation of furfural (FU) was investigated over Fe-containing MgO catalysts, on a continuous gas flow reactor, using methanol as a hydrogen donor. Catalysts were prepared either by coprecipitation or impregnation methods, with different Fe/Mg atomic ratios. The main product was 2-methylfuran (MFU), an important highly added value chemical, up to 92% selectivity. The catalyst design helped our understanding of the impact of acid/base properties and the nature of iron species in terms of catalytic performance. In particular, the addition of iron on the surface of the basic oxide led to (i) the increase of Lewis acid sites, (ii) the increase of the dehydrogenation capacity of the presented catalytic system, and (iii) to the significant enhancement of the FU conversion to MFU. FTIR studies, using methanol as the chosen probe molecule, indicated that, at the low temperature regime, the process follows the typical hydrogen transfer reduction, but at the high temperature regi...

Research paper thumbnail of Hydrogen Transfer Activation via Stabilization of Coordinatively Vacant Sites: Tuning Long-Range π-System Electronic Interaction between Ru(0) and NHC Pendants

Research paper thumbnail of A cascade mechanism for a simple reaction: The gas-phase methylation of phenol with methanol

Research paper thumbnail of Mg/Ga mixed-oxide catalysts for phenol methylation: Outstanding performance in 2,4,6-trimethylphenol synthesis with co-feeding of water

Applied Catalysis A: General

Research paper thumbnail of Catalytic Bio-Refining of Ethanol from Wine Waste to Butanol and Higher Alcohols: Modeling the Life Cycle Assessment and Process Design

ACS Sustainable Chemistry & Engineering

Research paper thumbnail of Ethanol aerobic and anaerobic oxidation with FeVO4 and V2O5 catalysts

Applied Catalysis A: General

Research paper thumbnail of Hard-template preparation of Au/CeO2 mesostructured catalysts and their activity for the selective oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid

Microporous and Mesoporous Materials, 2016

Research paper thumbnail of Adsorbent-Adsorbate Interactions in the Oxidation of HMF Catalyzed by Ni-Based MOFs: A DRIFT and FT-IR Insight

The Journal of Physical Chemistry C, 2016

Research paper thumbnail of Pt�Sn/?-Al 2O 3 and Pt�Sn�Na/?-Al 2O 3 catalysts for hydrogen production by dehydrogenation of Jet A

Fuel and Energy Abstracts, 2011

Research paper thumbnail of Vanadium and niobium mixed-oxide catalysts obtained via sol-gel: preparation and catalytic behaviour in oxidative dehydrogenation of propane

Studies in Surface Science and Catalysis, 2005

... Dalton Trans. 291 (1973) [22] JM Amarilla, B. Casal and E. Ruiz-Hitzky, Mater. Lett. 8 (1989)... more ... Dalton Trans. 291 (1973) [22] JM Amarilla, B. Casal and E. Ruiz-Hitzky, Mater. Lett. 8 (1989) 132 [23] AA McConnell, JS Anderson and CNR Rao, Spectrochim. Acta 32A (1976) 1067. ... Mater. Lett., 8 (1989), p. 132. [23] AA McConnell, JS Anderson and CNR Rao. Spectrochim. ...

Research paper thumbnail of The control of selectivity in rutile-type Sn/V/Nb/Sb mixed oxides catalysts for propane ammoxidation through a variation of the Sb content

Research paper thumbnail of Sol–Gel synthesis and characterization of Nb-Mo and Nb-Mo-V mixed oxides as potential catalysts for the selective oxidation of propane

Studies in Surface Science and Catalysis, 2006

In this work a modified hydrolytic sol-gel technique has been applied to synthesize binary and te... more In this work a modified hydrolytic sol-gel technique has been applied to synthesize binary and ternary systems based on Nb, Mo and V, as potential catalysts for the selective oxidation of propane to acrolein and/or acrylic acid. Crystalline mixed oxide phases were obtained and investigate by XRD, Raman and UV-VIS spectroscopy.

Research paper thumbnail of Insights into the reaction mechanism for 5-hydroxymethylfurfural oxidation to FDCA on bimetallic Pd–Au nanoparticles

Applied Catalysis A: General, 2014

ABSTRACT This work deals with the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarbox... more ABSTRACT This work deals with the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) in water using supported Pd–Au nanoparticles. The active phase composition was shown to be crucial for FDCA formation. Indeed, both Au and Pd monometallic nanoparticles formed 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) under the studied conditions; however, with Pd nanoparticles HMFCA was not further transformed, while Au and bimetallic Pd–Au systems both catalysed its oxidation to FDCA.

Research paper thumbnail of The Gas-Phase Ammoxidation of n-Hexane to Unsaturated C6 Dinitriles, Intermediates for Hexamethylenediamine Synthesis

Chemical Industries, 2008

This chapter reports about an investigation on the catalytic gas-phase ammoxidation of n-hexane a... more This chapter reports about an investigation on the catalytic gas-phase ammoxidation of n-hexane aimed at the production of 1,6-C 6 dinitriles, precursors for the synthesis of hexamethylenediamine. Catalysts tested were those also active and selective in the ammoxidation of propane to acrylonitrile: rutile-type V/Sb and Sn/V/Nb/Sb mixed oxides. Several N-containing compounds formed; however, the selectivity to cyanocontaining aliphatic linear C 6 compounds was low, due to the relevant contribution of side reactions such as combustion, cracking and formation of heavy compounds.

Research paper thumbnail of Insights into the reaction mechanism for 5-hydroxymethylfurfural oxidation to FDCA on bimetallic Pd–Au nanoparticles

ABSTRACT This work deals with the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarbox... more ABSTRACT This work deals with the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) in water using supported Pd–Au nanoparticles. The active phase composition was shown to be crucial for FDCA formation. Indeed, both Au and Pd monometallic nanoparticles formed 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) under the studied conditions; however, with Pd nanoparticles HMFCA was not further transformed, while Au and bimetallic Pd–Au systems both catalysed its oxidation to FDCA.

Research paper thumbnail of Steam reforming of clean biogas over Rh and Ru open-cell metallic foam structured catalysts

Research paper thumbnail of Biogas to Syngas through the Combined Steam/Dry Reforming Process: An Environmental Impact Assessment

Research paper thumbnail of Effect of exchange procedure and crystal size on high silica MFI zeolite as catalyst for vapor phase Beckmann rearrangement

Studies in Surface Science and Catalysis

ABSTRACT Caprolactam is the starting monomer for the production of Nylon-6 fibers and resins. The... more ABSTRACT Caprolactam is the starting monomer for the production of Nylon-6 fibers and resins. The current caprolactam manufacturing process is energy intensive and generates considerable wastes (ammonium sulphate). For this reason, alternative paths for the production of caprolactam providing few-step cost effective production and environmentally friendly process are required. In year 2000 Sumitomo Inc. announced the build-up of a demonstration plant for the production of caprolactam.. This process allows an ammonium sulphate-free caprolactam manufacture and will result in an industrial plant by the end of year 2003. In a recent paper Ichihashi et al. [1]claimed long-time catalytic tests with a high silica MFI zeolite which is rather active and selective towards caprolactam production. In this paper we report a study on the effect of catalyst activation method and acid sites distribution on caprolactam selectivity of high silica MFI zeolites of different crystal size. We found that catalysts activation by a NH4NO3 alkaline solution and calcinations at 450°C promotes structural rearrangement of silicalite-1 unit cell and catalytic performances remarkably higher than other silicalite-1 activated by other methods. In addition we show the direct correlation between caprolactam selectivity and H-bonded (nests of silanols and vicinal silanols) distribution.

Research paper thumbnail of Urea and Polyurea Production: An Innovative Solvent- and Catalyst-Free Approach through Catechol Carbonate

ACS Sustainable Chemistry & Engineering

Research paper thumbnail of The competition between dehydrogenation and dehydration reactions for primary and secondary alcohols over gallia: unravelling the effects of molecular and electronic structure via a two-pronged theoretical/experimental approach

Catalysis Science & Technology

The relative dehydrogenation/dehydration reactivity imparted by nanostructured gallium(iii) oxide... more The relative dehydrogenation/dehydration reactivity imparted by nanostructured gallium(iii) oxide on alcohols was investigated via electronic structure calculations, reactivity tests and DRIFT-IR spectroscopy.

Research paper thumbnail of Tandem Hydrogenation/Hydrogenolysis of Furfural to 2-Methylfuran over a Fe/Mg/O Catalyst: Structure–Activity Relationship

Catalysts

The hydrodeoxygenation of furfural (FU) was investigated over Fe-containing MgO catalysts, on a c... more The hydrodeoxygenation of furfural (FU) was investigated over Fe-containing MgO catalysts, on a continuous gas flow reactor, using methanol as a hydrogen donor. Catalysts were prepared either by coprecipitation or impregnation methods, with different Fe/Mg atomic ratios. The main product was 2-methylfuran (MFU), an important highly added value chemical, up to 92% selectivity. The catalyst design helped our understanding of the impact of acid/base properties and the nature of iron species in terms of catalytic performance. In particular, the addition of iron on the surface of the basic oxide led to (i) the increase of Lewis acid sites, (ii) the increase of the dehydrogenation capacity of the presented catalytic system, and (iii) to the significant enhancement of the FU conversion to MFU. FTIR studies, using methanol as the chosen probe molecule, indicated that, at the low temperature regime, the process follows the typical hydrogen transfer reduction, but at the high temperature regi...

Research paper thumbnail of Hydrogen Transfer Activation via Stabilization of Coordinatively Vacant Sites: Tuning Long-Range π-System Electronic Interaction between Ru(0) and NHC Pendants

Research paper thumbnail of A cascade mechanism for a simple reaction: The gas-phase methylation of phenol with methanol

Research paper thumbnail of Mg/Ga mixed-oxide catalysts for phenol methylation: Outstanding performance in 2,4,6-trimethylphenol synthesis with co-feeding of water

Applied Catalysis A: General

Research paper thumbnail of Catalytic Bio-Refining of Ethanol from Wine Waste to Butanol and Higher Alcohols: Modeling the Life Cycle Assessment and Process Design

ACS Sustainable Chemistry & Engineering

Research paper thumbnail of Ethanol aerobic and anaerobic oxidation with FeVO4 and V2O5 catalysts

Applied Catalysis A: General

Research paper thumbnail of Hard-template preparation of Au/CeO2 mesostructured catalysts and their activity for the selective oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid

Microporous and Mesoporous Materials, 2016

Research paper thumbnail of Adsorbent-Adsorbate Interactions in the Oxidation of HMF Catalyzed by Ni-Based MOFs: A DRIFT and FT-IR Insight

The Journal of Physical Chemistry C, 2016

Research paper thumbnail of Pt�Sn/?-Al 2O 3 and Pt�Sn�Na/?-Al 2O 3 catalysts for hydrogen production by dehydrogenation of Jet A

Fuel and Energy Abstracts, 2011

Research paper thumbnail of Vanadium and niobium mixed-oxide catalysts obtained via sol-gel: preparation and catalytic behaviour in oxidative dehydrogenation of propane

Studies in Surface Science and Catalysis, 2005

... Dalton Trans. 291 (1973) [22] JM Amarilla, B. Casal and E. Ruiz-Hitzky, Mater. Lett. 8 (1989)... more ... Dalton Trans. 291 (1973) [22] JM Amarilla, B. Casal and E. Ruiz-Hitzky, Mater. Lett. 8 (1989) 132 [23] AA McConnell, JS Anderson and CNR Rao, Spectrochim. Acta 32A (1976) 1067. ... Mater. Lett., 8 (1989), p. 132. [23] AA McConnell, JS Anderson and CNR Rao. Spectrochim. ...

Research paper thumbnail of The control of selectivity in rutile-type Sn/V/Nb/Sb mixed oxides catalysts for propane ammoxidation through a variation of the Sb content

Research paper thumbnail of Sol–Gel synthesis and characterization of Nb-Mo and Nb-Mo-V mixed oxides as potential catalysts for the selective oxidation of propane

Studies in Surface Science and Catalysis, 2006

In this work a modified hydrolytic sol-gel technique has been applied to synthesize binary and te... more In this work a modified hydrolytic sol-gel technique has been applied to synthesize binary and ternary systems based on Nb, Mo and V, as potential catalysts for the selective oxidation of propane to acrolein and/or acrylic acid. Crystalline mixed oxide phases were obtained and investigate by XRD, Raman and UV-VIS spectroscopy.

Research paper thumbnail of Insights into the reaction mechanism for 5-hydroxymethylfurfural oxidation to FDCA on bimetallic Pd–Au nanoparticles

Applied Catalysis A: General, 2014

ABSTRACT This work deals with the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarbox... more ABSTRACT This work deals with the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) in water using supported Pd–Au nanoparticles. The active phase composition was shown to be crucial for FDCA formation. Indeed, both Au and Pd monometallic nanoparticles formed 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) under the studied conditions; however, with Pd nanoparticles HMFCA was not further transformed, while Au and bimetallic Pd–Au systems both catalysed its oxidation to FDCA.

Research paper thumbnail of The Gas-Phase Ammoxidation of n-Hexane to Unsaturated C6 Dinitriles, Intermediates for Hexamethylenediamine Synthesis

Chemical Industries, 2008

This chapter reports about an investigation on the catalytic gas-phase ammoxidation of n-hexane a... more This chapter reports about an investigation on the catalytic gas-phase ammoxidation of n-hexane aimed at the production of 1,6-C 6 dinitriles, precursors for the synthesis of hexamethylenediamine. Catalysts tested were those also active and selective in the ammoxidation of propane to acrylonitrile: rutile-type V/Sb and Sn/V/Nb/Sb mixed oxides. Several N-containing compounds formed; however, the selectivity to cyanocontaining aliphatic linear C 6 compounds was low, due to the relevant contribution of side reactions such as combustion, cracking and formation of heavy compounds.

Research paper thumbnail of Insights into the reaction mechanism for 5-hydroxymethylfurfural oxidation to FDCA on bimetallic Pd–Au nanoparticles

ABSTRACT This work deals with the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarbox... more ABSTRACT This work deals with the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) in water using supported Pd–Au nanoparticles. The active phase composition was shown to be crucial for FDCA formation. Indeed, both Au and Pd monometallic nanoparticles formed 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) under the studied conditions; however, with Pd nanoparticles HMFCA was not further transformed, while Au and bimetallic Pd–Au systems both catalysed its oxidation to FDCA.