Faculty of Natural Sciences

TY - JOUR

T1 - Towards Solid-State Magnesium Batteries

T2 - Ligand-Assisted Superionic Conductivity

AU - Skov, Lasse Najbjerg

AU - Grinderslev, Jakob

AU - Rosenkranz, Asger Wulff

AU - Lee, Young-Su

AU - Jensen, Torben René

PY - 2022/9

Y1 - 2022/9

N2 - Solid-state inorganic magnesium batteries are considered as potential high energy storage devices of the future. Here we present a series of magnesium borohydride tetrahydrofuran (THF) composites, Mg(BH 4) 2 ⋅ xTHF(−MgO), 0≤x≤3, as solid-state electrolytes for magnesium batteries. Three new monoclinic compounds were identified, Mg(BH 4) 2 ⋅ 2/3THF (Cc), α-Mg(BH 4) 2 ⋅ 2THF (P2 1/c) and β-Mg(BH 4) 2 ⋅ 2THF (C2), and the detailed structures of α- and β-Mg(BH 4) 2 ⋅ 2THF are presented. The magnesium ionic conductivity of composites formed by these compounds were several orders of magnitude higher than that of the distinct compounds, x=0, 2/3, 2, and 3. The nanocomposite stabilized by MgO nanoparticles (∼50 nm), Mg(BH 4) 2 ⋅ 1.5THF−MgO(75 wt%), displayed the highest Mg 2+ conductivity, σ(Mg 2+)∼10 −4 S cm −1 at 70 °C, a high ionic transport number of t ion=0.99, and cyclic voltammetry revealed an oxidative stability of ∼1.2 V vs. Mg/Mg 2+. The electrolyte was stable towards magnesium electrodes, which allowed for stable Mg plating/stripping for at least 100 cycles at 55 °C with a current density of 0.1 mA cm −2. Finally, a proof-of-concept rechargeable solid-state magnesium battery was assembled with a magnesium metal anode and a TiS 2 cathode. A maximum discharge capacity of 94.2 mAh g −1 was displayed, which corresponds to y=0.2 in Mg yTiS 2.

AB - Solid-state inorganic magnesium batteries are considered as potential high energy storage devices of the future. Here we present a series of magnesium borohydride tetrahydrofuran (THF) composites, Mg(BH 4) 2 ⋅ xTHF(−MgO), 0≤x≤3, as solid-state electrolytes for magnesium batteries. Three new monoclinic compounds were identified, Mg(BH 4) 2 ⋅ 2/3THF (Cc), α-Mg(BH 4) 2 ⋅ 2THF (P2 1/c) and β-Mg(BH 4) 2 ⋅ 2THF (C2), and the detailed structures of α- and β-Mg(BH 4) 2 ⋅ 2THF are presented. The magnesium ionic conductivity of composites formed by these compounds were several orders of magnitude higher than that of the distinct compounds, x=0, 2/3, 2, and 3. The nanocomposite stabilized by MgO nanoparticles (∼50 nm), Mg(BH 4) 2 ⋅ 1.5THF−MgO(75 wt%), displayed the highest Mg 2+ conductivity, σ(Mg 2+)∼10 −4 S cm −1 at 70 °C, a high ionic transport number of t ion=0.99, and cyclic voltammetry revealed an oxidative stability of ∼1.2 V vs. Mg/Mg 2+. The electrolyte was stable towards magnesium electrodes, which allowed for stable Mg plating/stripping for at least 100 cycles at 55 °C with a current density of 0.1 mA cm −2. Finally, a proof-of-concept rechargeable solid-state magnesium battery was assembled with a magnesium metal anode and a TiS 2 cathode. A maximum discharge capacity of 94.2 mAh g −1 was displayed, which corresponds to y=0.2 in Mg yTiS 2.

KW - magnesium batteries

KW - solid electrolytes

KW - magnesium conductors

KW - nanocomposites

U2 - 10.1002/batt.202200163

DO - 10.1002/batt.202200163

M3 - Journal article

VL - 5

JO - Batteries & Supercaps

JF - Batteries & Supercaps

SN - 2566-6223

IS - 9

M1 - e202200163

ER -