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1.
ChemSusChem ; 17(1): e202301063, 2024 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-37671901

RESUMO

Vanadium redox flow battery (VRFB) electrodes face challenges related to their long-term operation. We investigated different electrode treatments mimicking the aging processes during operation, including thermal activation, aging, soaking, and storing. Several characterization techniques were used to deepen the understanding of the treatment of carbon felts. Synchrotron X-ray imaging, electrochemical impedance spectroscopy (EIS) with the distribution of relaxation times analysis, and dynamic vapor sorption (DVS) revealed differences between the wettability of felts. The bulk saturation after electrolyte injection into the carbon felts significantly differed from 8 % to 96 %. DVS revealed differences in the sorption/desorption behavior of carbon felt ranging from a slight change of 0.8 wt % to over 100 wt %. Additionally, the interactions between the water vapor and the sample change from type V to type H2. After treatment, morphology changes were observed by atomic force microscopy and scanning electron microscopy. Cyclic voltammetry and EIS were used to probe the electrochemical performance, revealing different catalytic activities and transport-related impedances for the treated samples. These investigations are crucial for understanding the effects of treatments on the performance and optimizing materials for long-term operation.

2.
ACS Appl Mater Interfaces ; 15(40): 46775-46789, 2023 Oct 11.
Artigo em Inglês | MEDLINE | ID: mdl-37768857

RESUMO

Carbon electrodes are one of the key components of vanadium redox flow batteries (VRFBs), and their wetting behavior, electrochemical performance, and tendency to side reactions are crucial for cell efficiency. Herein, we demonstrate three different types of electrode modifications: poly(o-toluidine) (POT), Vulcan XC 72R, and an iron-doped carbon-nitrogen base material (Fe-N-C + carbon nanotube (CNT)). By combining synchrotron X-ray imaging with traditional characterization approaches, we give thorough insights into changes caused by each modification in terms of the electrochemical performance in both half-cell reactions, wettability and permeability, and tendency toward the hydrogen evolution side reaction. The limiting performance of POT and Vulcan XC 72R could mainly be ascribed to hindered electrolyte transport through the electrode. Fe-N-C + CNT displayed promising potential in the positive half-cell with improved electrochemical performance and wetting behavior but catalyzed the hydrogen evolution side reaction in the negative half-cell.

3.
Chem Commun (Camb) ; 57(20): 2547-2550, 2021 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-33585854

RESUMO

Understanding the interaction of phosphoric acid and porous electrocatalysts is of vital importance for a rational design of high performance phosphoric acid based fuel cells on a molecular level. We demonstrate for the first time that NMR spectroscopy can be used for elucidating the preferred distribution sites of phosphoric acid in various nanoporous carbons. A pore size dependent negative chemical shift of 31P is observed, serving as a distinct signature of pore occupation, and applied for analysing a commercial catalyst (Pt@Vulcan) as a practical application.

4.
ChemSusChem ; 13(12): 3154-3165, 2020 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-32286001

RESUMO

The wetting behavior and affinity to side reactions of carbon-based electrodes in vanadium redox flow batteries (VRFBs) are highly dependent on the physical and chemical surface structures of the material, as well as on the cell design itself. To investigate these properties, a new cell design was proposed to facilitate synchrotron X-ray imaging. Three different flow geometries were studied to understand the impact on the flow dynamics, and the formation of hydrogen bubbles. By electrolyte injection experiments, it was shown that the maximum saturation of carbon felt was achieved by a flat flow field after the first injection and by a serpentine flow field after continuous flow. Furthermore, the average saturation of the carbon felt was correlated to the cyclic voltammetry current response, and the hydrogen gas evolution was visualized in 3D by X-ray tomography. The capabilities of this cell design and experiments were outlined, which are essential for the evaluation and optimization of cell components of VRFBs.

5.
Materials (Basel) ; 9(12)2016 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-28774092

RESUMO

One of the problems that arise with bifluoride- or fluoride-containing compounds is their poor solubility in non-aqueous solvents. We report herein a facile one-pot synthesis and the chemical analysis of fluoride/bifluoride-containing polymers, which are soluble in MeCN. Different polymers, such as Polyvinylacetate or Polyethylene imine and saccharides, such as maltodextrin, were complexed with ammonium (bi)fluoride using hydrogen bonds to form the desired (bi)fluoride-containing compounds. The newly formed hydrogen bonding (bi)fluoride-doped polymer matrices were analyzed using infrared and nuclear magnetic resonance spectroscopies, and X-ray diffraction. The promising materials also underwent impedance spectroscopy, conductivity measurements and preliminary tests as electrolytes for room temperature fluoride ion batteries along with an analysis of their performance.

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