The influence of physical parameters on the in-situ metal carbonyl complex formation studied with the Fast On-line Reaction Apparatus (FORA)

Wittwer, Yves; Eichler, Robert; Herrmann, Dominik; Türler, Andreas

doi:10.1515/ract-2020-0035

Cited by 2 publications

(1 citation statement)

References 44 publications

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“…Recent systematic studies of all involved experimental parameters using the Fast On-line Reaction Apparatus (FORA) revealed a number of possibilities on how to further increase the formation and transport yields of MCCs. [50] Therefore, even experiments with the heavier transactinide elements Bh as well as Hs and Mt are within reach upon solid preparation. vacuum chromatography [58] to predict the required temperature scales.…”

Section: A Roadmap To the Futurementioning

confidence: 99%

Radiochemical Research with Transactinide Elements in Switzerland

Steinegger

Eichler

2020

Chimia

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Here, we present a review on a fundamental radiochemical research topic performed by Swiss scientists in national and international collaborations, utilizing large accelerator facilities at the Paul Scherrer Institute as well as abroad. The chemical investigation of the heaviest elements of the periodic table is a truly multidisciplinary effort, which allows scientists to venture into a variety of fields ranging from nuclear and radiochemistry to experimental and theoretical work in inorganic and physical chemistry all the way to nuclear and atomic physics. The structure and fundamental ordering scheme of all elements in the periodic table, as established more than 150 years ago, is at stake: The ever increasing addition of new elements at the heavy end of the periodic table together with a growing influence of relativistic effects, raises the question of how much periodicity applies in this region of the table. Research on the heaviest chemical elements requires access to large heavy-ion accelerator facilities as well as to rare actinide isotopes as target materials. Thus, this scientific area is inevitably embedded in joint international efforts. Its fundamental character ensures academic relevance and thereby substantially contributes to the future of nuclear sciences in Switzerland.

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Section: A Roadmap To the Futurementioning

confidence: 99%

Radiochemical Research with Transactinide Elements in Switzerland

Steinegger

Eichler

2020

Chimia

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The influence of gas purification and addition of macro amounts of metal-carbonyl complexes on the formation of single-atom metal-carbonyl-complexes

et al. 2021

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Using the Fast On-line Reaction Apparatus (FORA), the influence of various gas-purification columns onto the formation of metal carbonyl complexes (MCCs) under single-atom chemistry conditions was investigated. MCCs were synthesized from single atoms of Mo, Tc, Ru and Rh being produced by the spontaneous fission of 252Cf and recoiling into a CO-gas containing carrier gas atmosphere. The in-situ synthesized MCCs were volatile enough to be transported by the carrier gas to a charcoal trap where they were adsorbed and their subsequent decay was registered by γ-spectrometry. It was found that the type and combination of purification columns used to clean the applied CO-gas strongly influences the obtained formation and transport yields for all MCCs. With the exception of Rh-carbonyl, intense gas-purification strategies resulted in reduced formation and transport yields for MCCs in comparison with less efficient or even completely missing purification setups. It was postulated that the observed reduction in yield might depend on the content of Fe(CO)5 and Ni(CO)4, as well as potentially other MCCs, in the CO-gas, being formed by the interaction between CO and the steel-surfaces of FORA as well as from impurities in the used charcoal traps. Subsequently, it was shown that macro amounts of Fe(CO)5, Ni(CO)4, Mo(CO)6 and Re2(CO)10 added to the used process gas indeed increase significantly the overall yields for MCCs produced by 252Cf fission products. Ni(CO)4 appeared the most potent to increase the yield. Therefore, it was used in more detailed investigations. Using isothermal chromatography, it was shown that Ni(CO)4 does not affect the speciation of carbonyl species produced by the 252Cf fission product 104Mo. For 107Tc, 110Ru and 111Rh a speciation change cannot be excluded. For 111Rh a speciation change cannot be excluded. An inter-carbonyl transfer mechanism is suggested boosting the formation of MCCs. The current discovery might allow for new opportunities in various research fields, which are currently restricted by the low overall yields for MCCs produced under single-atom chemistry conditions. Examples are the chemical investigation of transactinides or the generation of radioactive ion beams from refractory metals at accelerators.

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The influence of physical parameters on the in-situ metal carbonyl complex formation studied with the Fast On-line Reaction Apparatus (FORA)

Cited by 2 publications

References 44 publications

Radiochemical Research with Transactinide Elements in Switzerland

Radiochemical Research with Transactinide Elements in Switzerland

The influence of gas purification and addition of macro amounts of metal-carbonyl complexes on the formation of single-atom metal-carbonyl-complexes

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