Lithiating magneto-ionics in a rechargeable battery

Abstract

Magneto-ionics, real-time ionic control of magnetism in solid-state materials, promise ultralow-power memory, computing, and ultralow-field sensor technologies. The real-time ion intercalation is also the key state-of-charge feature in rechargeable batteries. Here, we report that the reversible lithiation/delithiation in molecular magneto-ionic material, the cathode in a rechargeable lithium-ion battery, accurately monitors its real-time state of charge through a dynamic tunability of magnetic ordering. The electrochemical and magnetic studies confirm that the structural vacancy and hydrogen-bonding networks enable reversible lithiation and delithiation in the magnetic cathode. Coupling with microwave-excited spin wave at a low frequency (0.35 GHz) and a magnetic field of 100 Oe, we reveal a fast and reliable built-in magneto-ionic sensor monitoring state of charge in rechargeable batteries. The findings shown herein promise an integration of molecular magneto-ionic cathode and rechargeable batteries for real-time monitoring of state of charge.

Highly cyclable voltage control of magnetism in cobalt ferrite nanopillars for memory and neuromorphic applications

“…Ions that have been commonly explored include O 2− , H + , Li + , or ARTICLE scitation.org/journal/apm N 3− , [4][5][6][7] and they are introduced into the magnetic materials either from a solid or from a liquid electrolyte. [8][9][10][11][12][13] A high electric field at a magnetic material electrode-electrolyte interface (resulting from the formation of the electrical double-layer, EDL) acts as the driving force for ion migration. 14 As magneto-ionic systems are voltage-controlled rather than current-controlled, they are energy efficient with potential writing energies as low as ∼10 −3 fJ = 1 aJ.…”

Voltage Control of Multiple Electrochemical Processes during Lithium Ion Migration in NiFe2O4 Ferrite

“…Despite many efforts to investigate the electrochemical mechanisms, most research has focused on revealing a single mechanism of lithiation/delithiation. For example, magnetic and electrical manipulation driven by Li-ion intercalation and deintercalation at high voltage range has been widely reported while maintaining the crystal structure intact. , Redox conversion during the insertion or extraction of Li-ions is another important mechanism that enables a complete phase change. , In addition, a mechanism called space charge has emerged at low voltage to elucidate the origin of extra storage capacity in transition metal oxide Li-ion batteries. , Because of different voltage ranges, all three Li-ion modulation mechanisms, i.e ., intercalation, conversion, and space charge, can occur in a single material. However, a systematic study among the three electrochemical mechanisms within a same material in full voltage range is lacking.…”

“…For example, magnetic and electrical manipulation driven by Li-ion intercalation and deintercalation at high voltage range has been widely reported while maintaining the crystal structure intact. 5,6 Redox conversion during the insertion or extraction of Li-ions is another important mechanism that enables a complete phase change. 7,8 In addition, a mechanism called space charge has emerged at low voltage to elucidate the origin of extra storage capacity in transition metal oxide Li-ion batteries.…”

Molecular magneto-ionic proton sensor in solid-state proton battery

“…Magneto-ionic control of magnetic materials is based on the ionic motion and electrochemical reactions activated by external voltage 1,2 . In recent years, we have witnessed the successful ion control of magnetic properties for inorganic and molecule-based magnets from the strong coupling between ion and spin polarization, offering immense promise for developing magneto-ionic-based sensors [1][2][3][4][5][6][7] . In this context, molecular materials with porous and vacancy networks particularly attract significant interests due to its stimuli responsive magnetism.…”

“…In this context, molecular materials with porous and vacancy networks particularly attract significant interests due to its stimuli responsive magnetism. For example, lithium control of magnetism in moleculebased magnet has been integrated with rechargeable lithium-ion batteries for real-time state-of-charge estimation 7 . However, alkali metal ions typically show a limited diffusion rate in molecular materials due to its relatively large ionic radii.…”