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Projects / Programmes source: ARIS

Multidisciplinary approach towards development of a novel multifunctional heterogeneous catalyst for efficient conversion of H2 and CO2 gas mixtures into fuel additives and surrogates

Research activity

Code Science Field Subfield
2.02.00  Engineering sciences and technologies  Chemical engineering   

Code Science Field
T350  Technological sciences  Chemical technology and engineering 

Code Science Field
2.04  Engineering and Technology  Chemical engineering  
Keywords
heterogeneous catalysis, nanostructured catalysts, reaction kinetics and mechanisms, computer modelling, fuel additives, methanol, higher alcohols
Evaluation (rules)
source: COBISS
Researchers (12)
no. Code Name and surname Research area Role Period No. of publicationsNo. of publications
1.  17283  Špela Božič    Technical associate  2018 - 2021  38 
2.  28557  PhD Petar Djinović  Chemical engineering  Researcher  2018 - 2021  243 
3.  36345  PhD Dunja Gustinčič  Chemistry  Junior researcher  2018  20 
4.  53850  PhD Rohini Ashokrao Khobragade  Chemistry  Researcher  2020 - 2021  19 
5.  16188  PhD Anton Kokalj  Chemistry  Researcher  2018 - 2021  377 
6.  08027  PhD Antonija Lesar  Chemistry  Researcher  2018  121 
7.  01290  PhD Ingrid Milošev  Chemistry  Researcher  2018 - 2021  689 
8.  11874  PhD Albin Pintar  Chemical engineering  Head  2018 - 2021  850 
9.  37480  PhD Matic Poberžnik  Chemistry  Researcher  2018 - 2020  59 
10.  52492  PhD Vikram Sagar Tatiparthi  Chemistry  Researcher  2020 - 2021  40 
11.  38311  PhD Janvit Teržan  Chemical engineering  Junior researcher  2018 - 2020  73 
12.  32927  PhD Gregor Žerjav  Chemical engineering  Researcher  2018 - 2021  190 
Organisations (2)
no. Code Research organisation City Registration number No. of publicationsNo. of publications
1.  0104  National Institute of Chemistry  Ljubljana  5051592000  21,496 
2.  0106  Jožef Stefan Institute  Ljubljana  5051606000  90,010 
Abstract
Considering the facts that reserves of fossil fuels are rapidly diminishing, while we are at the same time witnessing a growing demand for energy and fuels, it is obvious that we need to reduce our dependence on fossil fuels and also the emission of greenhouse gases (CO2, CH4, N2O, etc.) with gradual transition to renewable sources, biofuels and wastes. The development of an appropriate heterogeneous catalyst that will actively and selectively convert mixtures of CO2 and H2 to methanol as a liquid fuel additive or surrogate, can significantly contribute to a more widespread large scale utilization of CO2. The main goal of the proposed basic research project is to develop a transition metal based catalyst which will contain appropriate active centers that enable direct conversion of CO2 and H2 to methanol (CH3OH) with a weight time yield of at least 2000 g methanol/(kgcat h) at 50 bar. The expected single pass methanol selectivity is above 75 % at 10 % CO2 conversion. To efficiently carry out catalytic direct CO2-to-methanol transformation, we will synthesize multifunctional mesoporous catalysts with high BET specific surface area (to expose a maximal number of active surface sites) by utilizing advanced catalyst preparation procedures. The synthesis of these solids will be based on Cu and ZnO active phases which will be promoted either by abundant transition metals such as iron (Fe) or rare earth metals exhibiting various oxidation states such as indium (In) and gallium (Ga). The role of the reducible oxophyllic rare earth elements will be stabilization of the partly hydrogenated CO2Hx intermediates which are crucial for high methanol selectivity. Also, the morphology and chemical composition of the catalyst will be tailored towards minimization of simultaneously occurring methanol steam reforming reaction (MeOH+H2O → CO2+3H2), which results in a loss of MeOH yield. The synthesized catalyst samples will be thoroughly characterized by a variety of relevant characterization techniques. Moreover, in situ and operando spectroscopic techniques will be utilized to both optimize catalyst surface properties and investigate in detail the reaction mechanism. Activity and selectivity of synthesized catalysts in the process of direct CO2-to-methanol transformation will be studied in a fixed-bed tubular laboratory-scale reactor system running in a wide range of reaction conditions (180-300°C, 10-80 bar, WHSV between 40-400 L/(gcat h), systematic variation of H2 and CO2 feed concentrations). In this way we will obtain detailed kinetic data for the investigated reaction and isolate the most suitable catalyst formulation. An emphasis will be given to investigate and determine quantitative structure-activity and structure-selectivity relationships (QSAR). Finally, long-term experiments of the optimal catalyst composition will be performed. The theoretical DFT approach will be employed to study the modes of H2 and CO2 activation on the catalysts as a function of active site geometry, presence of transition metal or rare earth dopants. Also, identification of the plausible reaction intermediates and the energy barriers for the individual reaction steps will be evaluated. This information will act either for supporting the experimental findings or for identification of possible kinetic bottlenecks and their remediation through redesign of a catalyst. A comprehensive documentation will be prepared, which will allow for a future design of a pilot plant unit enabling methanol production of 1 g/min (which corresponds to volumetric gas feed rate of carbon dioxide of approximately 10 L/min at the goal conversion and selectivity).
Significance for science
Currently available knowledge in the field of catalytic transformation of carbon dioxide and hydrogen to methanol is deficient, especially in terms of synthesis of such heterogeneous catalysts, which would enable efficient (i.e. active and selective) synthesis of the product from reactants. This knowledge will be enriched on the basis of literature data and in particular on the basis of knowledge and experience gained through the realization of proposed basic research project. Within the scope of this project we will synthesize an advanced and multifunctional heterogeneous catalyst, which will enable long-term operation of reactor units and thus to effectively and economically conduct catalytic transformation of carbon dioxide and hydrogen to methanol as a fuel additive. The content of the proposed basic research project is original in the following areas: (1) novel and advanced catalytic materials will be synthesized and tested that will allow efficient (active and selective) hydrogenation of carbon dioxide to methanol; (2) the final product (developed catalyst) will have the appropriate characteristics for a direct use; (3) the reactor system for catalytic transformation of carbon dioxide and hydrogen to methanol will be designed accordingly to the previously isolated optimal catalyst. In the field of catalytic transformation of carbon dioxide and hydrogen to methanol we will significantly expand body of knowledge, regarding the design of appropriate catalysts and their effective application in the real process. Subsequently, this will certainly upgrade the existing knowledge of chemical engineering discipline, too. Knowledge gained during the implementation of the proposed basic research project, will enable much simpler and more efficient exploitation of carbon dioxide from various sources, which are now largely ignored and exploited very inefficiently. The principal method of disseminating the results will be through published papers in leading refereed international journals devoted to energy, catalysis and chemical engineering as well as in patent literature. The mechanism by which transfer of knowledge will take place involves presentations at national and international conferences and contributions to databases. To illustrate the benefits of the project to key stakeholders in the field of catalysis, other target groups and to the general public, we will take advantage of different communication tools, such as preparation of digital brochures and regular updating of webpage. The project proposal is fully aligned with the Slovenia’s Smart Specialisation Strategy (S4), adopted by the Government of Slovenia on 20.. 9. 2015. Aims of S4 are to strengthen the competitiveness of the economy by enhancing its innovation capacity, diversify existing industries and service activities and boost growth of new and fast growing industries and enterprises. The proposal with a clear focus on advanced materials will be an ideal partner to bridge the research community with industrial environment.
Significance for the country
Currently available knowledge in the field of catalytic transformation of carbon dioxide and hydrogen to methanol is deficient, especially in terms of synthesis of such heterogeneous catalysts, which would enable efficient (i.e. active and selective) synthesis of the product from reactants. This knowledge will be enriched on the basis of literature data and in particular on the basis of knowledge and experience gained through the realization of proposed basic research project. Within the scope of this project we will synthesize an advanced and multifunctional heterogeneous catalyst, which will enable long-term operation of reactor units and thus to effectively and economically conduct catalytic transformation of carbon dioxide and hydrogen to methanol as a fuel additive. The content of the proposed basic research project is original in the following areas: (1) novel and advanced catalytic materials will be synthesized and tested that will allow efficient (active and selective) hydrogenation of carbon dioxide to methanol; (2) the final product (developed catalyst) will have the appropriate characteristics for a direct use; (3) the reactor system for catalytic transformation of carbon dioxide and hydrogen to methanol will be designed accordingly to the previously isolated optimal catalyst. In the field of catalytic transformation of carbon dioxide and hydrogen to methanol we will significantly expand body of knowledge, regarding the design of appropriate catalysts and their effective application in the real process. Subsequently, this will certainly upgrade the existing knowledge of chemical engineering discipline, too. Knowledge gained during the implementation of the proposed basic research project, will enable much simpler and more efficient exploitation of carbon dioxide from various sources, which are now largely ignored and exploited very inefficiently. The principal method of disseminating the results will be through published papers in leading refereed international journals devoted to energy, catalysis and chemical engineering as well as in patent literature. The mechanism by which transfer of knowledge will take place involves presentations at national and international conferences and contributions to databases. To illustrate the benefits of the project to key stakeholders in the field of catalysis, other target groups and to the general public, we will take advantage of different communication tools, such as preparation of digital brochures and regular updating of webpage. The project proposal is fully aligned with the Slovenia’s Smart Specialisation Strategy (S4), adopted by the Government of Slovenia on 20.. 9. 2015. Aims of S4 are to strengthen the competitiveness of the economy by enhancing its innovation capacity, diversify existing industries and service activities and boost growth of new and fast growing industries and enterprises. The proposal with a clear focus on advanced materials will be an ideal partner to bridge the research community with industrial environment.
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