Application of a novel gas phase synthesis approach to carbonyl complexes of accelerator-produced 5d transition metals

2021 ◽  
Vol 0 (0) ◽  
Author(s):  
Michael Götz ◽  
Alexander Yakushev ◽  
Stefan Götz ◽  
Antonio Di Nitto ◽  
Christoph E. Düllmann ◽  
...  

Abstract In 2014 the first synthesis of a transactinide carbonyl complex – seaborgium hexacarbonyl – was reported. This was achieved in gas-phase chemical experiments in a beam-free environment behind the recoil separator GARIS. Extending this work to heavier elements requires more efficient techniques to synthesize carbonyl complexes as production rates of transactinide elements drop with increasing atomic number. A novel approach was thus conceived, which retains the benefit of a beam-free environment but avoids the physical preseparation step. The latter reduces the yields for products of asymmetric reactions such as those used for the synthesis of suitable isotopes of Sg, Bh, Hs and Mt. For this a series of experiments with accelerator-produced radioisotopes of the lighter homologues W, Re and Os was carried out at the tandem accelerator of JAEA Tokai, Japan. A newly developed double-chamber system, which allows for a decoupled recoil ion thermalization and chemical complex formation, was used, which avoids the low-efficiency physical preseparation step. Here, we demonstrate the feasibility of this newly developed method using accelerator-produced short-lived radioisotopes of the 5d homologues of the early transactinides.

2021 ◽  
Vol 0 (0) ◽  
Author(s):  
Michael Götz ◽  
Stefan Götz ◽  
Jens-Volker Kratz ◽  
Jochen Ballof ◽  
Christoph E. Düllmann ◽  
...  

Abstract The formation of carbonyl complexes using atom-at-a-time quantities of short-lived transition metals from fusion and fission reactions was reported in 2012. Numerous studies focussing on this chemical system, which is also applicable for the superheavy elements followed. We report on a novel two-chamber approach for the synthesis of such complexes that allows spatial decoupling of thermalization and gas-phase carbonyl complex synthesis. Neutron induced fission on 235U and spontaneous fission of 248Cm were employed for the production of the fission products. These were stopped inside a gas volume behind the target and flushed with an inert-gas flow into a second chamber. This was flushed with carbon monoxide to allow the gas-phase synthesis of carbonyl complexes. Parameter studies of the transfer from the first into the second chamber as well as on the carbonyl complex formation and transport processes have been performed. High overall efficiencies of more than 50% were reached rendering this approach interesting for studies of superheavy elements. Our results show that carbonyl complex formation of thermalized fission products is a single-atom reaction, and not a hot-atom reaction.


2012 ◽  
Vol 1405 ◽  
Author(s):  
Dan A. Kaplowitz ◽  
Jason Jouet ◽  
Michael R. Zachariah

ABSTRACTWe show a low temperature gas-phase synthesis route to produce faceted aluminum crystals in the aerosol phase. Use of triisobutylaluminum whose decomposition temperature is below the melting point of elemental aluminum enabled us to grow nanocrystals from its vapor. Combustion tests show an increase in energy release compared to commercial nanoaluminum. Production of aluminum in an oxygen free environment resulted in a bare aluminum surface that was passivated in separate experiments with nickel and iron by decomposition of their carbonyl precursors.


2021 ◽  
Vol 109 (4) ◽  
pp. 243-260 ◽  
Author(s):  
Yves Wittwer ◽  
Robert Eichler ◽  
Dominik Herrmann ◽  
Andreas Türler

Abstract A new setup named Fast On-line Reaction Apparatus (FORA) is presented which allows for the efficient investigation and optimization of metal carbonyl complex (MCC) formation reactions under various reaction conditions. The setup contains a 252Cf-source producing short-lived Mo, Tc, Ru and Rh isotopes at a rate of a few atoms per second by its 3% spontaneous fission decay branch. Those atoms are transformed within FORA in-situ into volatile metal carbonyl complexes (MCCs) by using CO-containing carrier gases. Here, the design, operation and performance of FORA is discussed, revealing it as a suitable setup for performing single-atom chemistry studies. The influence of various gas-additives, such as CO2, CH4, H2, Ar, O2, H2O and ambient air, on the formation and transport of MCCs was investigated. O2, H2O and air were found to harm the formation and transport of MCCs in FORA, with H2O being the most severe. An exception is Tc, for which about 130 ppmv of H2O caused an increased production and transport of volatile compounds. The other gas-additives were not influencing the formation and transport efficiency of MCCs. Using an older setup called Miss Piggy based on a similar working principle as FORA, it was additionally investigated if gas-additives are mostly affecting the formation or only the transport stability of MCCs. It was found that mostly formation is impacted, as MCCs appear to be much less sensitive to reacting with gas-additives in comparison to the bare Mo, Tc, Ru and Rh atoms.


ChemInform ◽  
2001 ◽  
Vol 32 (8) ◽  
pp. no-no
Author(s):  
A. Zak ◽  
Y. Feldman ◽  
V. Alperovich ◽  
R. Rosentsveig ◽  
R. Tenne

Nano Letters ◽  
2008 ◽  
Vol 8 (7) ◽  
pp. 2012-2016 ◽  
Author(s):  
Albert Dato ◽  
Velimir Radmilovic ◽  
Zonghoon Lee ◽  
Jonathan Phillips ◽  
Michael Frenklach

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