ORCID Profile
0000-0002-2320-6111
Current Organisation
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
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Publisher: American Chemical Society (ACS)
Date: 25-07-2014
DOI: 10.1021/JP5023339
Abstract: Solute-solvent electronic structure interactions of iron porphyrin at very low concentration in dichloromethane (CH2Cl2) liquid solution are reported. Two iron porphyrin complexes are investigated here-iron octaethylporphyrin chloride (FeOEP-Cl) and iron tetraphenylporphyrin chloride (FeTPP-Cl)-using X-ray absorption and emission spectroscopy at the Fe L2,3 edge, and spectra are interpreted with the help of density functional theory/restricted open-shell configuration interaction singles (DFT/ROCIS) calculations. It is argued that the Fe center of FeOEP-Cl is more capable of binding small solvent molecules, exemplified here for Cl2CH2, than FeTPP-Cl in solution. The proposed binding mechanism is through the assistance of the dipole interaction between the porphyrin-ligand system and the solvent molecule, in a situation where the ligand structure and arrangement maximize the binding interactions. Our studies demonstrate that even small ligands, depending on their structure and arrangement, can have considerable effects on porphyrin's metal center chemistry in liquid solution.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4NR06639A
Abstract: The electronic structure of nanodiamonds, probed by soft X-ray absorption and emission spectroscopies, is found to change upon aqueous dispersion.
Publisher: Wiley
Date: 20-06-2018
Abstract: MnO
Publisher: Wiley
Date: 21-01-2015
Abstract: Changes in the local electronic structure of the Mn 3d orbitals of a Mn catalyst derived from a dinuclear Mn(III) complex during the water oxidation cycle were investigated ex situ by X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS) analyses. Detailed information about the Mn 3d orbitals, especially the local HOMO-LUMO gap on Mn sites revealed by RIXS analyses, indicated that the enhancement in catalytic activity (water oxidation) originated from the narrowing of the local HOMO-LUMO gap when electrical voltage and visible light illumination were applied simultaneously to the Mn catalytic system.
Publisher: Informa UK Limited
Date: 04-03-2017
Publisher: American Chemical Society (ACS)
Date: 06-08-2014
DOI: 10.1021/JP505129M
Abstract: Resonant inelastic X-ray scattering spectra at the iron L-edge from hemin in dimethyl sulfoxide liquid solution are reported. Our experiments, which are interpreted with the help of electronic structure calculations, support earlier assignments of hemin-solvent interactions, including the iron spin state and the role of the chloride ligand obtained from a total fluorescence yield study. The analysis of the explicit radiative relaxation channels of 2p core-level excited iron, explored in the present work, allows for a rather quantitative assignment of the orbitals involved in the excitation-deexcitation process of the core-excited hemin in solution. We specifically distinguish between contributions of partially and fully occupied valence orbitals to the broad X-ray emission band. In addition, our calculations reveal a detailed picture of the character of these orbitals.
Publisher: Wiley
Date: 06-02-2019
Publisher: Wiley
Date: 15-06-2021
Abstract: The instability and expense of anodes for water electrolyzers with acidic electrolytes can be overcome through the implementation of a cobalt‐iron‐lead oxide electrocatalyst, [Co–Fe–Pb]O x , that is self‐healing in the presence of dissolved metal precursors. However, the latter requirement is pernicious for the membrane and especially the cathode half‐reaction since Pb 2+ and Fe 3+ precursors poison the state‐of‐the‐art platinum H 2 evolving catalyst. To address this, we demonstrate the invariably stable operation of [Co–Fe–Pb]O x in acidic solutions through a cobalt‐selective self‐healing mechanism without the addition of Pb 2+ and Fe 3+ and investigate the kinetics of the process. Soft X‐ray absorption spectroscopy reveals that low concentrations of Co 2+ in the solution stabilize the catalytically active Co(Fe) sites. The highly promising performance of this system is showcased by steady water electrooxidation at 80±1 °C and 10 mA cm −2 , using a flat electrode, at an overpotential of 0.56±0.01 V on a one‐week timescale.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4CP04703F
Abstract: The local electronic structure of the cobalt centre-ion of Co( iii ) protoporphyrin IX chloride dissolved in dimethyl sulfoxide (DMSO) liquid solution is studied by resonant inelastic X-ray scattering (RIXS) spectroscopy at the cobalt L-edge.
Publisher: Wiley
Date: 06-02-2019
Abstract: Manganese oxide (MnO
Publisher: Wiley
Date: 15-06-2021
Abstract: The instability and expense of anodes for water electrolyzers with acidic electrolytes can be overcome through the implementation of a cobalt‐iron‐lead oxide electrocatalyst, [Co–Fe–Pb]O x , that is self‐healing in the presence of dissolved metal precursors. However, the latter requirement is pernicious for the membrane and especially the cathode half‐reaction since Pb 2+ and Fe 3+ precursors poison the state‐of‐the‐art platinum H 2 evolving catalyst. To address this, we demonstrate the invariably stable operation of [Co–Fe–Pb]O x in acidic solutions through a cobalt‐selective self‐healing mechanism without the addition of Pb 2+ and Fe 3+ and investigate the kinetics of the process. Soft X‐ray absorption spectroscopy reveals that low concentrations of Co 2+ in the solution stabilize the catalytically active Co(Fe) sites. The highly promising performance of this system is showcased by steady water electrooxidation at 80±1 °C and 10 mA cm −2 , using a flat electrode, at an overpotential of 0.56±0.01 V on a one‐week timescale.
Location: Germany
No related grants have been discovered for Jie Xiao.