The study of rhenium pentacarbonyl complexes using single-atom chemistry in the gas phase

2019 ◽  
Vol 21 (13) ◽  
pp. 7147-7154
Author(s):  
Yang Wang ◽  
Shiwei Cao ◽  
Jicai Zhang ◽  
Fangli Fan ◽  
Jie Yang ◽  
...  
Keyword(s):  
Gas Phase ◽  
Single Atom ◽  
Atom Level ◽  
Atom Chemistry

Two experiments prove Re pentacarbonyl could exist stably in the gas phase at the single-atom level.

scholarly journals The influence of chemical parameters on the in-situ metal carbonyl complex formation studied with the fast on-line reaction apparatus (FORA)

2021 ◽  
Vol 109 (4) ◽  
pp. 243-260 ◽  
Author(s):  
Yves Wittwer ◽  
Robert Eichler ◽  
Dominik Herrmann ◽  
Andreas Türler
Keyword(s):  
Metal Carbonyl ◽  
Ambient Air ◽  
Single Atom ◽  
Carbonyl Complex ◽  
Carbonyl Complexes ◽  
On Line ◽  
Carrier Gases ◽  
And Performance ◽  
Atom Chemistry

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.

Vacuum Chromatography of Tl on SiO2 at the Single-Atom Level

2016 ◽  
Vol 120 (13) ◽  
pp. 7122-7132 ◽  
Author(s):  
Patrick Steinegger ◽  
Masato Asai ◽  
Rugard Dressler ◽  
Robert Eichler ◽  
Yusuke Kaneya ◽  
...  
Keyword(s):  
Single Atom ◽  
Atom Level

scholarly journals Atomic Electron Tomography: Probing 3D Structure and Material Properties at the Single-Atom Level

2017 ◽  
Vol 23 (S1) ◽  
pp. 1886-1887
Author(s):  
Yongsoo Yang ◽  
Chien-Chun Chen ◽  
M. C. Scott ◽  
Colin Ophus ◽  
Rui Xu ◽  
...  
Keyword(s):  
Material Properties ◽  
Electron Tomography ◽  
3D Structure ◽  
Atomic Electron ◽  
Single Atom ◽  
Atom Level

Single-atom electron microscopy for energy-related nanomaterials

2020 ◽  
Vol 8 (32) ◽  
pp. 16142-16165 ◽  
Author(s):  
Mingquan Xu ◽  
Aowen Li ◽  
Meng Gao ◽  
Wu Zhou
Keyword(s):  
Electron Microscopy ◽  
Transmission Electron Microscopy ◽  
Scanning Transmission Electron Microscopy ◽  
Atomic Resolution ◽  
Single Atom ◽  
Transmission Electron ◽  
Scanning Transmission ◽  
Resolution Imaging ◽  
Imaging And Spectroscopy ◽  
Atom Level

The advances in aberration correction have enabled atomic-resolution imaging and spectroscopy in scanning transmission electron microscopy (STEM) under low primary voltages and pushed their detection limit down to the single-atom level.

scholarly journals Imaging Nucleation, Growth and Disorder at the Single-atom Level by Atomic Electron Tomography (AET)

2020 ◽  
Vol 26 (S2) ◽  
pp. 1848-1850
Author(s):  
Peter Ercius ◽  
Jihan Zhou ◽  
Yongsoo Yang ◽  
Yao Yang ◽  
Dennis Kim ◽  
...  
Keyword(s):  
Electron Tomography ◽  
Atomic Electron ◽  
Single Atom ◽  
Atom Level ◽  
Nucleation Growth

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

2021 ◽  
Vol 0 (0) ◽  
Author(s):  
Yves Wittwer ◽  
Robert Eichler ◽  
Ronald Zingg ◽  
Dominik Herrmann ◽  
Andreas Türler
Keyword(s):  
Metal Carbonyl ◽  
Fission Products ◽  
Single Atom ◽  
Gas Purification ◽  
Carbonyl Complexes ◽  
Carrier Gas ◽  
Metal Carbonyl Complexes ◽  
Process Gas ◽  
Atom Chemistry ◽  
Co Gas

Abstract 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.

On The Nature of Interstellar Organic Chemistry

1997 ◽  
Vol 161 ◽  
pp. 89-96 ◽  
Author(s):  
Steven B. Charnley
Keyword(s):  
Gas Phase ◽  
Molecular Clouds ◽  
Organic Molecules ◽  
Single Atom ◽  
Addition Reactions ◽  
Mass Star ◽  
Quantum Tunnelling ◽  
Dark Clouds ◽  
Murchison Meteorite ◽  
Low Mass

AbstractA theory for the origin of all organic molecules observed in regions of massive and low-mass star formation, as well as in dark molecular clouds is described. On dust grains, single atom addition reactions and stability of the intermediate radicals, mechanisms similar to those believed to form the organic component of the Murchison meteorite, lead to a very limited number of mantle compositions depending upon the degree of hydrogenation. The key step in the theory is the formation of the formyl radical by H atom addition (by quantum tunnelling) to CO. Subsequent H atom additions lead to formaldehyde and methanol, as previously suggested; C, N, and O atoms can also undergo additions to HCO. For increasing hydrogenation, the mantle types include one in which there is little contribution from formyl-initiated chemistry; one in which an acetylenic chain develops through C atom additions; and others where the acetylenic chain is increasingly hydrogenated to form aldehydes and alcohols. Following evaporation of grain mantles, such as occurs in protostellar «hot cores», these molecules can form new organics, for example, by alkyl cation transfer from alcohols. In dark clouds, different mantles lead to different gas phase organics. This scenario accounts naturally for the formation of many interstellar organics for which none presently exists, predicts observable correlations between specific interstellar molecules, indicates the presence of many new organic molecules and why several others are not observed.

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