Abstract
Abstract The Fast On-line Reaction Apparatus (FORA) was used to investigate the influence of various reaction parameters onto the formation and transport of metal carbonyl complexes (MCCs) under single-atom chemistry conditions. FORA is based on a 252Cf-source producing short-lived Mo, Tc, Ru and Rh isotopes. Those are recoiling from the spontaneous fission source into a reaction chamber flushed with a gas-mixture containing CO. Upon contact with CO, fission products form volatile MCCs which are further transported by the gas stream to the detection setup, consisting of a charcoal trap mounted in front of a HPGe γ-detector. Depending on the reaction conditions, MCCs are formed and transported with different efficiencies. Using this setup, the impact of varying physical parameters like gas flow, gas pressure, kinetic energy of fission products upon entering the reaction chamber and temperature of the reaction chamber on the formation and transport yields of MCCs was investigated. Using a setup similar to FORA called Miss Piggy, various gas mixtures of CO with a selection of noble gases, as well as N2 and H2, were investigated with respect to their effect onto MCC formation and transport. Based on this measurements, optimized reaction conditions to maximize the synthesis and transport of MCCs are suggested. Explanations for the observed results supported by simulations are suggested as well.
Highlights
In 1890, the synthesis and identification of Ni(CO)4 by Ludwig Mond and Co-workers marked the beginning of a new class of chemical compounds, the metal carbonyl complexes (MCCs) [1]
Fast On-line Reaction Apparatus (FORA) was used to investigate the effects of gas flow, pressure, kinetic energy of fission products and temperature of the reaction chamber on the formation and transport of MCCs
According to the results presented here, high gas flows are desirable in any case, having a rather large impact on the overall yield for MCCs
Summary
In 1890, the synthesis and identification of Ni(CO) by Ludwig Mond and Co-workers marked the beginning of a new class of chemical compounds, the metal carbonyl complexes (MCCs) [1]. Since TAs were not found in nature up to today, they need to be produced in nuclear fusion reactions at a rate of a few atoms per day up to a few atoms per month depending on the investigated isotope Their half-lives are generally low, being usually in the range of a few seconds [8,9,10, 13, 14]. It became quickly apparent that the synthesis of MCCs under single-atom chemistry conditions goes along with low formation and transport yields. This was the case for heavy elements, and for their lighter homologous. To assist FORA, an older setup based on a similar principle, Miss Piggy [31], was used in some cases specified in the experimental section
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