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Electrolysis03:00

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In a galvanic cell, the electrical work is done by a redox system on its surroundings as electrons produced by the spontaneous redox reactions are transferred through an external circuit. Alternatively, an external circuit does work on a redox system by imposing a voltage sufficient to drive an otherwise nonspontaneous reaction in a process known as electrolysis. For instance, recharging a battery involves the use of an external power source to drive the spontaneous (discharge) cell reaction in...
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Electricity is generated by either electrons or ions flowing through a solution or a conducting medium. This flow of electrons or specifically electrical charge is defined as an electric current. When electrons move through a wire, they generate an electric current. It can be recalled  that in a redox reaction, electrons are lost and gained. In the spontaneous redox reaction of zinc  with copper, when zinc is immersed in a copper ion solution, a transfer of electrons from one...
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Spontaneous Chemical Reactions
Spontaneous redox reactions occur abundantly in nature. The chemical reaction occurring in a disposable AA battery powering our remote controls is one such example of a spontaneous redox reaction. Another example is the immersion of coiled copper wire into an aqueous silver nitrate solution. The reaction shows a gradual, visually impressive color change from colorless to bright blue and the formation of a grey precipitate on the copper wire. In this experiment,...
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Electrogravimetric analysis measures the weight of an analyte deposited electrolytically onto a suitable working electrode. This method involves applying a potential to a pre-weighed electrode submerged in a solution, which results in the desired substance being deposited through reduction at the cathode or oxidation at the anode. The electrode's weight is recorded after deposition, and the difference in weight gives the analyte's weight in the solution.
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Electrodeposition01:08

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Electrodeposition is a technique used to separate an analyte from interferents by electrochemical processes. Here, the analyte is a metal ion that can be deposited on an electrode immersed in the sample solution. The electrochemical setup consists of an anode and a cathode. When an electric current is applied to the setup, oxidation occurs at the anode. At the cathode, which consists of a large metal surface, metal ions undergo reduction and deposit onto the surface.
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Voltammetry: Overview01:20

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Voltammetry is an electroanalytical technique in which the current flowing through an electrochemical cell is measured as a function of applied potential, typically under conditions of concentration polarization. The technique provides valuable information about redox-active species, and the current response is plotted as a voltammogram.
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Reductive Electropolymerization of a Vinyl-containing Poly-pyridyl Complex on Glassy Carbon and Fluorine-doped Tin Oxide Electrodes
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Electrolyte Reactivity on the MgV2O4 Cathode Surface.

Heonjae Jeong1,2, Dan-Thien Nguyen1,3, Yingjie Yang1,4

  • 1The Joint Center for Energy Storage Research (JCESR), Argonne National Laboratory, Lemont, Illinois 60439, United States.

ACS Applied Materials & Interfaces
|October 8, 2023
PubMed
Summary
This summary is machine-generated.

Understanding electrolyte decomposition in magnesium batteries is key to preventing surface passivation. This study reveals that Mg2+ desolvation drives electrolyte breakdown on cathode surfaces, forming passivating fluorides.

Keywords:
Cathode-electrolyte interphase formationDensity functional theoryMgV2O4 cathodeion soft landingsurface reactivity

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Computational Chemistry

Background:

  • Electrode-electrolyte interface instabilities and surface passivation are major challenges in multivalent magnesium batteries.
  • Predicting molecular interactions and chemical reactivity of electrolyte components on electrode surfaces is crucial for battery performance.

Purpose of the Study:

  • To investigate the intrinsic reactivities of electrolyte species in magnesium bis(trifluoromethanesulfonimide) (Mg(TFSI)2) in diglyme (G2) on a magnesium vanadate (MgV2O4) cathode.
  • To elucidate the mechanisms of electrolyte decomposition at the electrode-electrolyte interface.

Main Methods:

  • First-principles calculations to study the adsorption and reactivity of electrolyte ions and molecules on MgV2O4.
  • Multimodal spectroscopy (X-ray photoelectron, X-ray absorption near-edge structure, electron energy-loss) and transmission electron microscopy.
  • Ion soft landing technique to create well-defined electrolyte-MgV2O4 interfaces for experimental analysis.

Main Results:

  • Nonsolvated [Mg(TFSI)]+ showed the strongest adsorption on MgV2O4, while partially solvated [Mg(TFSI):G2]+ was the most reactive.
  • Predicted C-S bond cleavage in TFSI- and C-O bond cleavage in G2 as dominant decomposition pathways, forming species like CF3- and CH3+.
  • Experimental results confirmed electrolyte decomposition and formation of MgF2 and carbonates, particularly with [Mg(TFSI):G2]+, corroborating theoretical predictions.

Conclusions:

  • Mg2+ desolvation at the MgV2O4 surface triggers electrolyte decomposition via adsorption and charge transfer, leading to fluoride passivation.
  • Surface-induced decomposition is favored over intrinsic gas-phase dissociation.
  • Designing anodically stable electrolytes requires systems that facilitate cation desolvation.