Alain Roucoux

Ecole Nationale Supérieure de Chimie de Rennes, Institut des Sciences Chimiques de Rennes, Department Member

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Alokmay Datta

Saha Institute of Nuclear Physics

Nicole Herbots

Arizona State University

Sergio Granados

Clark University

Cüneyt Arslan

Istanbul Technical University

Petra Reinke

University of Virginia

shivani R pandya

Parul university

Manuel J Lis

Universitat Politecnica de Catalunya

Traian CICONE

University Politehnica of Bucharest

Juan Antonio Gabaldón

Universitat de València

Kuppusami Parasuraman

Sathyabama University

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Papers by Alain Roucoux

Highly Selective and Multigram Hydrogenation of Citral into Citronellal by Palladium Nanoparticles in Water

ACS Sustainable Chemistry & Engineering, Apr 20, 2022

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Nanoparticles in Catalysis

Wiley eBooks, Apr 12, 2021

and the Spanish National Research Council. Prof. Garcia has been active in the field of heterogen... more and the Spanish National Research Council. Prof. Garcia has been active in the field of heterogeneous catalysis working with zeolites, mesoporous materials, metal organic frameworks, graphene and nanoparticles, particularly supported gold nanoparticles. He has published over 600 papers and has filed over 25 patents, two of them in industrial exploitation. Prof. Garcia is the 2016 Rey D. Jaime I award in New technologies, Doctor Honoris Causa from the University of Bucharest and the recipient of the 2011 Janssen-Cilag award given by the Spanish Royal Society of Chemistry and the 2008 Alpha Gold of the Spanish Society of Glass and Ceramics.

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Photocatalytic oxygen transfer as an innovative route for N2O upgrading

As concentration of nitrous oxide (N 2 O) keeps growing steeply in the atmosphere, upgrading this... more As concentration of nitrous oxide (N 2 O) keeps growing steeply in the atmosphere, upgrading this anthropogenic greenhouse gas as a potential oxygen transfer agent constitutes a real challenge to limit global warming and ozone layer depletion. Decomposition of N 2 O is mainly described under highly energy-consuming thermal activation, owing to its high stability and large activation barrier, making it kinetically inert. Herein, we demonstrate the controlled photocatalytic upgrading of N 2 O as an oxygen atom donor, releasing only dinitrogen (N 2 ) as a benign co-product. The doped Ag@TiO 2 photocatalyst specifically activates N 2 O for controlled oxidation of phosphines avoiding mineralization, under mild conditions (room temperature, 1 atm,  = 365 nm), as a proof-of-concept of the valorization of N 2 O as an oxygen transfer agent. The catalytic system is active and selective in various organic solvents, as well as innovatively in water, depending on the phosphine structure.

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Water soluble polymer–surfactant complexes-stabilized Pd(0) nanocatalysts: Characterization and structure–activity relationships in biphasic hydrogenation of alkenes and α,β-unsaturated ketones

Journal of Catalysis, Aug 1, 2016

A suitable approach to stabilize palladium nanoparticles in water as a green reaction medium for ... more A suitable approach to stabilize palladium nanoparticles in water as a green reaction medium for catalytic hydrogenation reactions is described. Supramolecular self-assemblies, obtained through the mixture of modified polyethyleneimines as amphiphilic polymers and water-soluble ammonium salts as surfactants, were used as efficient protective agents in the synthesis of Pd(0) nanospecies. The size and dispersion of the nanoparticles prepared with these original self-assemblies were characterized by TEM, SAXS and DLS techniques. The performances of the catalysts according to the polymer-surfactant mixtures were investigated in the hydrogenation of alkenes and α,β-unsaturated ketones in pure biphasic water/substrate medium, under mild conditions (room temperature and 1 bar H 2 ). The nanocatalysts showed efficient catalytic activities and selectivity towards C=C bonds. From investigations, the polymer-surfactant complexes act as cooperative protective agents and a pertinent structure-activity relationship was proposed based on the zeta-potential values and the catalytic activity of the resulting colloids.

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Unprecedented selective synthesis of imines by photo-oxidative coupling under N2O atmosphere

The synthesis of imines was unprecedently performed using nitrous oxide (N2O) as a highly selecti... more The synthesis of imines was unprecedently performed using nitrous oxide (N2O) as a highly selective oxidative agent for the photocatalytic homo-coupling of amines. In a similar way, unsymmetrical imines were produced through cross-coupling of amines with alcohols. Promisingly, this greenhouse gas showed excellent performances towards the target reactions when photocatalytically activated at atmospheric pressure, with silver photodeposited on titanium dioxide as catalyst. Relevantly, reactions under N2O atmosphere exhibited high conversion rates and turn-over frequencies, and higher selectivities than the ones carried out under a dioxygen atmosphere. Mechanisms for both reactions were proposed with release of nitrogen and water as benign byproducts.

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Open cell foam materials as Pd reservoirs for Suzuki–Miyaura coupling catalysis at ppb level

Reaction Chemistry and Engineering, 2023

For the Suzuki-Miyaura C-C coupling, it is well accepted that the active catalytic species in the... more For the Suzuki-Miyaura C-C coupling, it is well accepted that the active catalytic species in the liquid phase are leached from the solid palladium precursor. This was demonstrated for shaped solid Pd precursors which allows fixed-bed applications in flow chemistry. Yet, many interesting solid Pd precursors, including supported nanoparticles (NPs), are available as finely divided powders that cannot be used in fixed-bed reactors because of the too high pressure drop generated. In this work, open cell foam materials (OCF) are used as supports for Pd/C, Siliacat-Pd(0) and Pd(II)-DPP catalysts powders and Pd(0) NPs. The coupling of 4-iodoacetophenone with phenylboronic acid is used as a model reaction to evaluate the activity of leached species. Some experiments with other aryl halides are also reported. It is shown that all the catalytic foams are able to leach active species and that trace amounts in the range 30-300 ppb of Pd in solution are sufficient to carry out the reaction while maintaining a low pressure drop.

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Selective palladium nanoparticles-catalyzed hydrogenolysis of industrially targeted epoxides in water

Journal of Catalysis, Apr 1, 2021

HAL is a multi-disciplinary open access archive for the deposit and dissemination of scientific r... more HAL is a multi-disciplinary open access archive for the deposit and dissemination of scientific research documents, whether they are published or not. The documents may come from teaching and research institutions in France or abroad, or from public or private research centers. L'archive ouverte pluridisciplinaire HAL, est destinée au dépôt et à la diffusion de documents scientifiques de niveau recherche, publiés ou non, émanant des établissements d'enseignement et de recherche français ou étrangers, des laboratoires publics ou privés.

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New Trends in the Design of Metal Nanoparticles and Derived Nanomaterials for Catalysis

The purpose of this first chapter is to introduce the content of the book "Nanoparticles & Cataly... more The purpose of this first chapter is to introduce the content of the book "Nanoparticles & Catalysis: Advances in Synthesis and Applications". As suggested by the title, this book is fully dedicated to the new trends in research addressing the engineering of metal nanoparticles for their application in catalysis field. After general information on the position, interests and perspectives of this over growing domain that is nanocatalysis, a short overview of the fifteen chapters gathered is provided. The so-assembled data cover different domains of nanocatalysis both in terms of nature of the nanocatalysts developed (metal nanoparticles or derived composite materials) than ofvariety catalyses and reaction media studied. The reported applications deal with either nanocatalysis in solution conditions or in supported ones. The readers from academic or industrial communities will find in this book a basic

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Impact of the charge transfer process on the Fe2+/Fe3+distribution at Fe3O4 magnetic surface induced by deposited Pd clusters

Surface Science, Oct 1, 2021

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Remediation of Diethyl Phthalate in Aqueous Effluents with TiO2-Supported Rh0 Nanoparticles as Multicatalytic Materials

Catalysts, Sep 27, 2021

An innovative "domino" process, based on an arene hydrogenation followed by a photocatalytic step... more An innovative "domino" process, based on an arene hydrogenation followed by a photocatalytic step, was designed for the remediation of endocrine disrupting compounds, in highly concentrated aqueous effluents. The novelty relies on the use of TiO 2 -supported zerovalent Rh nanoparticles as multicatalytic materials (MCMs) for this two-step treatment, applied on diethyl phthalate, which is a model aromatic pollutant frequently present in aquatic environments. This nanocomposite advanced material, which was easily prepared by a green, wet impregnation methodology, proved to be active in the successive reactions, the reduction in the aromatic ring, and the photodegradation step. This sustainable approach offers promising alternatives in the case of photoresistive compounds.

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Dual photocatalytic effect of Ag/TiO2 site for the total reduction of N2O and selective oxidation of valuable alcohols

Nitrous oxide (N2O), an important greenhouse gas usually decomposed under harsh thermal condition... more Nitrous oxide (N2O), an important greenhouse gas usually decomposed under harsh thermal conditions, was completely reduced into climate neutral N2 and H2O under mild photocatalytic conditions, in the presence of alcohols as reducing agents. This reaction, which combines the synergistic removal of N2O and alcohols oxidation, was extended to the selective production of valuable ketones and aldehydes, using Ag/TiO2 as dual-reaction site.

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Highly selective synthesis of citronellal in water at multigram scale by Pd nanoparticles-catalyzed hydrogenation of citral

The synthesis of citronellal, an added-value chemical for perfumery, was carried out by selective... more The synthesis of citronellal, an added-value chemical for perfumery, was carried out by selective and green hydrogenation of citral into citronellal in water. Aqueous suspensions of spherical ammonium-capped palladium nanoparticles with sizes around 3nm selectively reduced the conjugated carbon-carbon double bond. An excellent selectivity of 95% in citronellal was achieved at complete conversion under mild reaction conditions on a realistic 2 g scale in water. The presence of potassium hydroxide proved crucial to control the selectivity and avoid other hydrogenation co-products. These optimized results were further extended to a 135 g substrate loading with a relevant turnover number (TON) of 10 000.

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Multigram Scale-up of the Selective Hydrogenation of α-Pinene with Ruthenium Nanoparticles in Water

ACS Sustainable Chemistry & Engineering, Mar 27, 2020

This paper presents the successful use of ruthenium nanoparticles, stabilized in water by ammoniu... more This paper presents the successful use of ruthenium nanoparticles, stabilized in water by ammonium surfactants, in the selective hydrogenation of -pinene and the first industrially reported scale-up of this catalyst on a multigram-scale. After designing the nanocatalyst at the lab scale, operational parameters (substrate/metal ratio, pressure and temperature) were identified and optimized in the scale-up. The -pinene hydrogenation process was operated with a 200 g batch, under 30 bar H 2 and at 110°C, with a complete conversion and a selectivity of 98% into cis-pinane within 4 h. The catalyst was easily recycled through a liquid-liquid biphasic approach for 5 reaction cycles to achieve a total turnover number (TTON) of 14000.

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Catalytically active nanoparticles stabilized by host–guest inclusion complexes in water

Chemical Communications, 2009

Tandem dehalogenation–hydrogenation reaction of halogenoarenes as model substrates of endocrine disruptors in water: Rhodium nanoparticles in suspension vs. on silica support

Applied Catalysis A-general, Feb 1, 2011

This paper focuses on the removal of mono- and poly-halogenated arenes, as model substrates of en... more This paper focuses on the removal of mono- and poly-halogenated arenes, as model substrates of endocrine disrupting compounds from aqueous effluents. The efficiency of catalysts based on metallic nanoparticles in the tandem dehalogenation–hydrogenation reaction as a pre-treatment for the remediation of organic halogenated pollutants was studied. Two catalytic systems – aqueous colloidal Rh0 dispersions and SiO2-supported Rh0 nanoparticles – were

Polyhydroxylated ammonium chloride salt: a new efficient surfactant for nanoparticles stabilisation in aqueous media. Characterization and application in catalysis

Dalton Transactions, 2009

A trihydroxyammonium chloride has proved to be an efficient protective agent for Rh(0) nanopartic... more

From Hydroxyalkylammonium Salts to Protected-Rh(0) Nanoparticles for Catalysis in Water: Comparative Studies of the Polar Heads

Topics in Catalysis, Jun 26, 2013

Simulation and optimization of the removal of toluene in air by ozonation with a catalytic open-cell foam

Chemical Engineering Research and Design, 2021

A heterogeneous catalyst, composed of an open-cell glass foam support impregnated with zerovalent... more A heterogeneous catalyst, composed of an open-cell glass foam support impregnated with zerovalent ruthenium nanoparticles (loading around 0.1 wt.%), was used to remove toluene in air by catalytic ozonation. Experiments with lab-designed 2-6 cm length and 1.6 cm diameter catalysts were performed. A model based on the Langmuir-Hinshelwood mechanism, coupled with mass transfer limitations and including competitive effects between toluene and ozone, was designed. It accurately fits experimental data gathered at various temperatures (30-90°C), gas velocities (0.0025-0.017 m.s-1) and inlet ozone concentrations (6.4-11.2 g.m-3). The removal of ozone and toluene was mainly ruled by the ozone concentration at low concentrations while the adsorption competition becomes significant at high ozone concentrations. Predictive simulations, at 1.0 g.m-3 inlet toluene concentration, were compared in terms of investment cost, operating cost and process performances. The results highlighted the complexity of the process, which involves antagonist aims between toluene removal and the design of a compact and energy-efficient reactor. With the best operating conditions (90°C and 46 g.m-3 ozone inlet concentration), the removal of toluene reached 88% (removal rate of J o u r n a l P r e-p r o o f 0.25 g.m-3 .s-1) with a high ozone degradation (97%) in a moderate reactor length of 0.11 m. These good performances associated to the low cost of the catalyst's synthesis make it an efficient alternative for the removal of pollutants from air.

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Novel and sustainable catalytic ruthenium-doped glass foam for thermocatalytic oxidation of volatile organic compounds: an experimental and modeling study

An open cell foam catalyst consisting of a glass foam support impregnated with zerovalent rutheni... more An open cell foam catalyst consisting of a glass foam support impregnated with zerovalent ruthenium nanoparticles (aiming to 0.1 wt %) without washcoating was used for the first time to remove several volatile organic compounds (VOCs) by thermocatalytic oxidation. At initial concentrations between and 2 g•m -3 and temperatures ranging from 100 to 350 °C, up to 100% of removal was achieved for the four VOCs tested. The ease of abatement of the VOCs with temperature had the following order: ethanol > acetone > toluene > heptane. The removal of ethanol was then modeled considering mass-transfer limitation, temperature dependency, and by-product formation. Full mineralization of ethanol can be achieved with a 30 cm length reactor at 150 °C and 0.010 m•s -1 . While the tortuous foam achieved efficient mass transfer, the process was still limited by this phenomenon highlighting that the efficiency of the catalyst could be improved at higher gas velocities.

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Catalytic Oxidation Processes for the Upgrading of Terpenes: State-of-the-Art and Future Trends

Catalysts, 2019

Terpenic olefins constitute a relevant platform of renewable molecules, which could be used as ke... more Terpenic olefins constitute a relevant platform of renewable molecules, which could be used as key intermediates for the perfumery, flavoring, and pharmaceutical industries. The upgrading of these cheap and available agro-resources through catalytic oxidation processes remains of great interest, leading to the formation of either epoxides via the oxidation of the olefinic bond or α,β-unsaturated ketones by the Csp3-H functionalization at the α-position of the double bond. This critical review summarizes some of the most relevant homogeneous or heterogeneous catalysts designed for the oxidation of some abundant terpenic olefins in the last decade (2008–2018).

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Highly Selective and Multigram Hydrogenation of Citral into Citronellal by Palladium Nanoparticles in Water

ACS Sustainable Chemistry & Engineering, Apr 20, 2022

Download

Nanoparticles in Catalysis

Wiley eBooks, Apr 12, 2021

Download

Photocatalytic oxygen transfer as an innovative route for N2O upgrading

Download

Water soluble polymer–surfactant complexes-stabilized Pd(0) nanocatalysts: Characterization and structure–activity relationships in biphasic hydrogenation of alkenes and α,β-unsaturated ketones

Journal of Catalysis, Aug 1, 2016

Download

Unprecedented selective synthesis of imines by photo-oxidative coupling under N2O atmosphere

Download

Open cell foam materials as Pd reservoirs for Suzuki–Miyaura coupling catalysis at ppb level

Reaction Chemistry and Engineering, 2023

Download

Selective palladium nanoparticles-catalyzed hydrogenolysis of industrially targeted epoxides in water

Journal of Catalysis, Apr 1, 2021

Download

New Trends in the Design of Metal Nanoparticles and Derived Nanomaterials for Catalysis

Download

Impact of the charge transfer process on the Fe2+/Fe3+distribution at Fe3O4 magnetic surface induced by deposited Pd clusters

Surface Science, Oct 1, 2021

Download

Remediation of Diethyl Phthalate in Aqueous Effluents with TiO2-Supported Rh0 Nanoparticles as Multicatalytic Materials

Catalysts, Sep 27, 2021

Download

Dual photocatalytic effect of Ag/TiO2 site for the total reduction of N2O and selective oxidation of valuable alcohols

Download

Highly selective synthesis of citronellal in water at multigram scale by Pd nanoparticles-catalyzed hydrogenation of citral

Download

Multigram Scale-up of the Selective Hydrogenation of α-Pinene with Ruthenium Nanoparticles in Water

ACS Sustainable Chemistry & Engineering, Mar 27, 2020

Download

Catalytically active nanoparticles stabilized by host–guest inclusion complexes in water

Chemical Communications, 2009

Tandem dehalogenation–hydrogenation reaction of halogenoarenes as model substrates of endocrine disruptors in water: Rhodium nanoparticles in suspension vs. on silica support

Applied Catalysis A-general, Feb 1, 2011

Polyhydroxylated ammonium chloride salt: a new efficient surfactant for nanoparticles stabilisation in aqueous media. Characterization and application in catalysis

Dalton Transactions, 2009

A trihydroxyammonium chloride has proved to be an efficient protective agent for Rh(0) nanopartic... more

From Hydroxyalkylammonium Salts to Protected-Rh(0) Nanoparticles for Catalysis in Water: Comparative Studies of the Polar Heads

Topics in Catalysis, Jun 26, 2013

Simulation and optimization of the removal of toluene in air by ozonation with a catalytic open-cell foam

Chemical Engineering Research and Design, 2021

Download

Novel and sustainable catalytic ruthenium-doped glass foam for thermocatalytic oxidation of volatile organic compounds: an experimental and modeling study

Download

Catalytic Oxidation Processes for the Upgrading of Terpenes: State-of-the-Art and Future Trends

Catalysts, 2019

Download

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