1.  Hydrogenation of fullerenes at extreme conditions.

The proposed method for synthesis of new materials was discovered during my work in France (IMRA-Europe) related to hydrogen storage. It is well known that C₆₀  can be hydrogenated using different methods  with formation of hydrofullerenes C₆₀H_x ( with X up to ~44).  Recently we found that prolonged reaction of hydrogen gas (50-120Bar) with C₆₀ at high temperature conditions results in collapse of cage structure with formation of unusual hydrocarbon molecules, namely polycyclic aromatic hydrocarbons (PAH) [1]. The research was continued in Umeå University during 2004-2005. It was realized that the synthesis method is very general: hydrogen at conditions reactive for carbon can serve as both fragmentation driving force and stabilization power for marginally stable molecules.  Since the result of reaction is a complex mixture, analysis of synthesized materials required application of advanced mass spectrometric methods.  The research rapidly expanded to collaboration between   research groups from USA, Germany,  Switzerland, Russia and Sweden.  As a result of this work several papers were published during 2004-2006 [2-7].  It is clear to the moment that new direction in material synthesis methods and fullerene science is developing from our initial publications.  Using skills and top level facilities of leading experts in the field of hydrofullerenes (Prof. Billups group)  and mass spectrometry (Prof. Marshall group, Y.Tsybin) the evidence for existence of fragmented fullerenes C_56-59 stabilized by hydrogen was obtained  [2,4,6]. Synthesis of new samples was performed in Stockholm University in 2004, (Prof. Dag Noreus group) [2].

Simultaneously, new report with very similar results (synthesis of C₅₈ derivative) but under fluorination of C₆₀ appeared in “Science” [8]. Synthesis of new fullerenes with even smaller cages, if achieved, will be breakthrough similar to original discovery of fullerenes and methods for their bulk production.

The synthesis of hydrofullerenes was also performed at extremely high pressure conditions (2 GPa) using facilities of Bayreuth University and financial support from EU "Research Infrastructures: Transnational Access" Program [3].

Finally, hydrofullerenes with different composition C60Hx synthesized by direct reaction with hydrogen gas at high temperature are now studied extensively in our group in collaboration with Thomas Wågberg and Prof. Dan Jonalds (Organic Chemistry).   Recently, we have been able to produce a material consisting of more than 90 % single C_2v isomer C₆₀H₁₈ without any purification of the material [5]. Currently the C₇₀H₃₆ is under investigation by different methods, fisrt of all by  NMR.

 

1.     A.V.Talyzin, Yu.Shul’ga,  A.Jacob, “Comparative study of hydrofullerides C60Hx synthesized by direct and catalytic  hydrogenation.”, Appl.Phys.A., 78, 1005–1010, (2004).

2.     A.V. Talyzin, Y. O. Tsybin, J. M. Purcell, T. M. Schaub,  Y. M. Shulga, D.Noreus, T. Sato,  A. Dzwilewski,  B. Sundqvist and A. G. Marshall, Time-Resolved Reaction of Hydrogen Gas with C60 at Elevated Pressure and Temperature: Hydrogenation and Cage Fragmentation, Accepted to J.Phys.Chem.A, 2006

3.      A.V.talyzin, A.Dzwilewski, B.Sundqvist, Y.O.Tsybin, J.M.Purcell, A.G.Marshall, Y.M.Shulga, C.McCamon, L.Dubrovinsky, “Hydrogenation of C₆₀ at 2 GPa pressure and high temperature.” Chemical Physics, accepted, 2006

4.      A.V. Talyzin, Yury O. Tsybin, Tanner M. Schaub, Philippe Mauron, Yury M. Shulga, Andreas Zьttel, Bertil Sundqvist, Alan G. Marshall, “Composition of Hydrofullerene Mixtures Produced by C₆₀ Reaction with Hydrogen Gas Revealed by High-Resolution Mass Spectrometry”,  J. Phys.Chem. B, 109(26); 12742-12747  (2005).

5.     T. Wågberg, D. Johnels, A. Peera, M. Hedenstrцm, Y. M. Schulga, Y. O. Tsybin, J. M. Purcell, A. G. Marshall, D. Noreus, T. Sato, and A. V. Talyzin, Selective synthesis of the C_3v-isomer of C₆₀H₁₈, Org. Lett, 7(25); 5557-5560 (2005) http://pubs.acs.org/cgi-bin/abstract.cgi/orlef7/2005/7/i25/abs/ol052175p.html

6.     A.V. Talyzin.; Tsybin, Y. O.; Peera, A. A.; Schaub, T. M.; Marshall, A. G.; Sundqvist, B.; Mauron, P.; Zuttel, A.; Billups, W. E., “Synthesis of C59Hx and C58Hx Fullerenes Stabilized by Hydrogen”, J. Phys. Chem. B., 109(12), (Letter), 5403-5405, (2005).        http://pubs.acs.org/cgi-bin/abstract.cgi/jpcbfk/2005/109/i12/abs/jp050364j.html

7.     A.V. Talyzin, B. Sundqvist, Y.M. Shulga, A.A. Peera, P. Imus and W.E. Billups, “Gentle fragmentation of C₆₀ by strong hydrogenation: a route to synthesizing new materials”, Chem. Phys. Lett., 400, 112-116 (2004).

8.     P. A. Troshin, A.G. Avent, A. D. Darwish, N. Martsinovich, A. K. Abdul-Sada, J. M. Street, and R. Taylor, Isolation of Two Seven-Membered Ring C58 Fullerene Derivatives: C58F17CF3 and C58F18  Science 2005, 309: 278-281