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Guczi L.,Institute of Isotope and Surface Chemistry of Hungary | Beck A.,Institute of Isotope and Surface Chemistry of Hungary | Paszti Z.,Institute for Research In Catalysis
Catalysis Today | Year: 2012

In this contribution the general rules and the exceptions in the area of gold catalysis are discussed in order to establish a correlation between the size of the catalytically active element and its reactivity towards different classes of substrate molecules. The general behaviour of gold is that it is inactive in massive form while it can be used as a highly active catalyst when downsized. Throughout this paper experimental data from different sources are collected to proof that - according to this general behaviour - small molecules (CO, NO, etc.) can be activated only on small nanoparticles or roughened Au(1 1 1) surfaces, whereas Au(1 1 1) single crystals or extended metal films are active in the reaction of large molecules. This observation defines the applicability area of gold nanoparticles and the activity of large gold surfaces, films or single crystals. The above effect can be modulated by interfacial interaction between gold species and active oxide either if gold is deposited directly on them or is supported on inactive oxides (such as model SiO 2/Si(1 0 0) or high surface area amorphous or mesoporous silica) with minute amounts of promoter oxide. The oxide may invoke electronic interaction and simultaneously the defect structure of oxides likely has a key issue in the formation and stabilization of Au nanoparticles. On the other hand, it turned out that in some cases - independently of the interface - the key issue is the available gold area of Au nanoparticles dictating the reaction rate of a substrate. © 2011 Elsevier B.V. All rights reserved.


Grant
Agency: Cordis | Branch: H2020 | Program: RIA | Phase: SPIRE-05-2015 | Award Amount: 4.42M | Year: 2015

TERRA project aims to develop, from TRL 3 to 5, a tandem electrocatalytic reactor (TER) coupling an oxidation reaction to a reduction reaction, with thus the great potential advantage of i) saving resources and energy (needed to produce the oxidant and reductants for the two separate reactions), and ii) intensify the process (reduce the nr. of steps, coupling two synthesis processes and especially eliminating those to prepare the oxidation and reduction agents). The proposal address one of SPIRE Roadmap Key Actions New ways of targeting energy input via electrochemical. The TER unit may be used in a large field of applications, but will be developed for a specific relevant case: the synthesis of PEF (PolyEthylene Furanoate), a next generation plastic. TERRA project aims to make a step forward in this process by coupling the FDCA and MEG synthesis in a single novel TER reactor, with relevant process intensification. Between the elements of innovation of the approach are: i) operation at higher T,P than conventional electrochemical devices for chemical manufacturing, ii) use of noble-metal-free electrocatalysts, iii) use of novel 3D-type electrodes to increase productivity, iv) use of electrode with modulation of activity, v) possibility to utilize external bias (from unused electrical renewable energy) to enhance flexibility of operations. In addition to scale-up reactor and test under environmental relevant conditions (TRL 5), the approach in TERRA project is to address the critical elements to pass from lab-scale experimentation to industrial prototype with intensified productivity. These developments are critical for a wider use of electrochemical manufacturing in chemical and process industries.


Grant
Agency: Cordis | Branch: FP7 | Program: JTI-CP-FCH | Phase: SP1-JTI-FCH.2013.2.4 | Award Amount: 3.81M | Year: 2014

The objective of the HELMETH project is the proof of concept of a highly efficient Power-to-Gas (P2G) technology with methane as a chemical storage and by thermally integrating high temperature electrolysis (SOEC technology) with methanation. This thermal integration balancing the exothermal and endothermal processes is an innovation with a high potential for a most energy-efficient storage solution for renewable electricity, without any practical capacity and duration limitation, since it provides SNG (Substitute Natural Gas) as a product, which is fully compatible with the existing pipeline network and storage infrastructure. The realisation of the P2G technology as proposed within HELMETH needs several development steps and HELMETH focuses on two main technical and socio-economic objectives, which have to be met in order to show the feasibility of the technology: Elaboration of the conditions / scenarios for an economic feasibility of the P2G process towards methane as chemical storage, without significantly deteriorating the CO2-balance of the renewable electricity. Demonstration of the technical feasibility of a conversion efficiency > 85 % from renewable electricity to methane, which is superior to the efficiency for the generation of hydrogen via conventional water electrolysis. Within HELMETH the main focus lies in the development of a complete pressurized P2G module consisting of a pressurized steam electrolyser module, which is thermally integrated with an optimized carbon dioxide methanation module. The HELMETH project will prove and demonstrate that: the conversion of renewable electricity into a storable hydrocarbon by high-temperature electrolysis is a feasible option, high temperature electrolysis and methanation can be coupled and thermally integrated towards highest conversion efficiencies by utilizing the process heat of the exothermal methanation reaction in the high temperature electrolysis process.


Grant
Agency: Cordis | Branch: FP7 | Program: CP-FP | Phase: NMP.2012.2.1-2 | Award Amount: 4.71M | Year: 2012

The Eco2CO2 project aims at exploiting a photo-electro-chemical (PEC) CO2 conversion route for the synthesis of methanol as a key intermediate for the production of fine chemicals (fragrances, flavourings, adhesives, monomers,) in a lignocellulosic biorefinery. A distinct improvement in the ecological footprint of the envisaged chemical industries will thus be achieved by: i) boosting the potential of lignocellulosic biorefineries by exploiting secondary by-products such as furfurals or lignin; ii) providing a small but non-negligible contribution to the reduction of CO2 release into the atmosphere by exploitation of sunlight as an energy source. The most crucial development in the project will be the development of a PEC reactor capable of converting CO2 into methanol by exploiting water and sun light with a targeted conversion efficiency exceeding 6%, with reference to wavelengths above 400 nm, and an expected durability of 10.000 h. The above specifications must be reached without using expensive noble metals or precious materials which should enable costs of the PEC panels lower than 60 Euro/m2 including the installation. Catalytic reactions of methanol and furfural to produce perfuming agents via partial oxidation or methylation, as well as of lignin or lignin depolymerisation derivatives to produce adhesives or monomers (e.g. p-xylene) will undergo a R&D programme to achieve cost effective production of green fine chemicals, proven by the end of the project via lab bench tests of at least 100 g/h production rates. Based on early calculations, if successful, the Eco2CO2 technologies should be capable of inducing avoided CO2 emissions by the year 2020 as high as 50 Mtons/year worldwide.


Grant
Agency: Cordis | Branch: FP7 | Program: CP-IP | Phase: NMP-2009-3.2-1 | Award Amount: 8.31M | Year: 2010

The project concept is to combine nanoreactor technology with multisite solid catalyst design to achieve a safer, cleaner and intensified chemical production. The project ideas are the following: (i) From micro- to nano-reactors. Actual microreactor have channels of micrometric size. We will develop a new concept based on the use of nanometric size channels. (ii) Vectorial pathway for multisite catalytic reactions. A limit in cascade (or domino) reactions is that there is no possibility to control the sequence of reactions of transformation of a reactant in a multisite catalyst. The concept of vectorial pathway for multisite catalytic reactions is based on the idea of an ordered sequence of catalytic sites along the axial direction of the channels of a membrane, in order to control the sequence of transformation. (iii) Dynamic nanoreactor. The concept of dynamic nanoreactor is based on the transient generation of toxic reactants inside the nanoreactor and the immediate conversion, in order to eliminate the storage of these reactants (which is minimized, but not eliminated in on-site or on-demand approaches). The project concept is that the implementation of innovative and safer pathways for sustainable chemical production requires making a step forward in the development of catalyst-reactor design along the lines indicated above. The project applies above ideas to three reactions of synthesis of large-volume chemicals which are relevant example of innovative pathways for sustainable chemical production: (1) direct synthesis of H2O2, (2) PO synthesis with in-situ generated H2O2 and (3) solvent-free synthesis of DPC with in-situ transient generation of phosgene. The consortium has a clear industrial leadership, with sixth major companies and two SMEs, and four academic partners, plus the participation of the durable institution of the NoE IDECAT.

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