Fundamental anionic, cat-ionic, and neutral atomic metal predictions utilizing density functional theory calculations validate the recent discovery identifying the interplay between the resonances and the RT minimum obtained through complex angular m
omentum analysis as the fundamental atomic mechanism underlying nano-scale catalysis. Here we investigate the optimization of the catalytic behavior of Au, Ag, Pd, Rh, and Os atomic systems via polarization effects and conclude that anionic atomic systems are optimal and therefore ideal for catalyzing the oxidation of water to peroxide, with anionic Os being the best candidate. The discovery that cat-ionic systems increase the transition energy barrier in the synthesis of peroxide could be important as inhibitors in controlling and regulating catalysis. These findings usher in a fundamental and comprehensive atomic theoretical framework for the generation of tun-able catalytic systems.
The catalytic activities of the atomic Y-, Ru-, At-, In-, Pd-, Ag-, Pt-, and Os- ions have been investigated theoretically using the atomic Au- ion as the benchmark for the selective partial oxidation of methane to methanol without CO2 emission. Disp
ersion-corrected density-functional theory has been used for the investigation. From the energy barrier calculations and the thermodynamics of the reactions, we conclude that the catalytic effect of the atomic Ag-, At-, Ru-, and Os- ions is higher than that of the atomic Au- ion catalysis of CH4 conversion to methanol. By controlling the temperature around 290K (Os-), 300K (Ag-), 310K (At-), 320K (Ru-) and 325K (Au-) methane can be completely oxidized to methanol without the emission of CO2. We conclude by recommending the investigation of the catalytic activities of combinations of the above negative ions for significant enhancement of the selective partial oxidation of methane to methanol.
We propose to use the near-threshold electron scattering data for atoms to guide the reliable experimental determination of their electron affinities (EAs), extracted using the Wigner Threshold Law, from laser photodetachment threshold spectroscopy m
easurements. Data from the near-threshold electron elastic scattering from W, Te, Rh, Sb and Sn atoms calculated using our complex angular momentum method, wherein is embedded the electron-electron correlations and core polarization interaction, are used as illustrations. We conclude with a remark on the relativistic effects on the EA calculation for the heavy At atom.
Bilodeau and Haugan [1], using Infrared laser photodetachment spectroscopy, measured the binding energies (BEs) of the ground state (4Fe9/2) and the excited state (4Fe7/2) of the Os^- ion to be 1.07780(12) eV and 0.553(3) eV, respectively. These valu
es are consistent with those calculated using Relativistic Configuration Interaction (RCI) calculations [2]. Here we have calculated the BEs for the ground state and the two excited states of the Os^- ion using our recent complex angular momentum (CAM) methodology [3] and obtained the BEs of 1.910, 1.230 and 0.224 eV, respectively (see Figure). We conclude that: 1) the measured value of 1.07780(12) eV corresponds to an excited state of Os^- and not to the EA of Os and 2) the EA of Os is 1.910 eV.
Low-energy E < 2 eV electron elastic collisions with Ge, Sn and Pb atoms yield stable excited Ge-, Sn- and Pb- anions. The recent Regge-pole methodology is used with Thomas-Fermi type potential incorporating the crucial core-polarization interaction
to calculate elastic total and Mulholland partial cross sections. For excited Ge- and Sn- anions the extracted binding energies from the unique characteristic sharp Regge resonances manifesting stable excited states formed during the collisions agree excellently with experimental values; for Pb- the prediction requires experimental verification. The calculated differential cross sections also yield the binding energies.
A novel method is proposed that uses very slow electron elastic collisions with atoms to identify their presence through the observation of tenuously bound (electron impact energy, E<0.1 eV) and weakly bound (E<1 eV) negative ions, formed as Regge resonances during the collisions.
