Catalysis and hydrogen storage subproject

subproject leader: Dr. Ágnes Kathó

I. Structure of the subproject

1. Catalysis WG

                 group leader: Dr. Ágnes Kathó

2. Hydrogen storage WG

               group leader: Dr. Gábor Papp

 II. Scientific goals

Synthesis of water-soluble transition metal complex catalysts (carbene- and tertiary phosphine-type ligands and Rh-, Ru-, Ir-, and Pd complexes thereof) and their application in reactions such as e.g. hydrogenation, hydrogen transfer, H-D-exchange, hydration of nitriles, C-C coupling and redox isomerization of alylic alcohols.

Application of the new catalysts in a)modification of biological membranes by hydrogenation, b)reactions with para-hydrogen for MRI purposes.

Catalytic hydrogenation of carbonates and bicarbonates to formates and catalytic decomposition of formates to yield hydrogen gas. Development of hydrogen storage systems based on  the reversible formate-bicarbonate transformation.

Development of environment-friedly catalytic processes (also with photochemical activation).

 III. Expected results

Elimination of the use of environment-contaminating organic solvents by a)development of high-activity catalyts suitable for application in aqueous media, b)development of solid-phase (solventless) reactions.

Useful transformations of biologically or environmentally relevant substrates, and development of environment-friendly catalytic technologies.

Development of new chemical hydrogen batteries for storage of energy from renewable sources  (in form of chemically bonded hydrogen) based on organometallic catalysis.

IV. Infrastucture

 Instruments to be purchased within the framework of the project:

 Glove box

Most of the planned reactions are catalyzed by oxygen-sensitive metal complexes. A glove box allows performing reactions in oxygen-free(and moisture-free) environment.

 Ball mill

Most chemical reactions take place in solvents which finally have to be removed (separated) from the target compounds and their regeneration also has to be solved. In some cases the solvent may induce side-reactions, too. Reactions which take place in solid phase during joint mechanical milling offer advantages over the traditional reactions using solvents. The ball mill is purchased for running such environment-friendly reactions.

 High volume Parr reactor

Rates and selectivities of chemical reactions are influenced by changes in pressure and/or temperature. The mentioned reactor allows safe processes at high temperature and pressure. For instance, in our reversible process for hydrogen storage, hydrogenation of bicarbonate requires high hydrogen pressure, while decomposition of formate may develop high hydrogen pressure, therefore the process requires the use of a high pressure reactor.

 Analytical HPLC

This is a high performance analytical tool for detection and identification of the products of many of our catalytic reactions. For example, in the research on hydrogen storage it is possible to follow the concentration of resulted or decomposed formate (in hydrogenation or dehydrogenation, respectively).

 High-pressure sapphire NMR tubes

These are indispensable for study of reactions under high gas pressure or those accompanied by increase of gas pressure. For example, in the various steps of hydrogen storage it is posssible to continuously determine the relative amounts of bicarbonate and formate and to establish the identity and structure of intermediates.

 Flow reactor

With the use of a flow reactor it is possible to study reactions in a short time in wide temperature and pressure ranges and by regulating the flow rate the residence time of the catalyst and reactants in the reactor can also be varied. An additional advantage is that only the active zone of the reactor requires heating, i.e. the energy requirement is low in comparison to batch reactions.