Transforming a Primary Li-SOCl₂ Battery into a High-Power Rechargeable System via Molecular Catalysis

Abstract

Li-SOCl 2 batteries possess ultrahigh energy densities and superior safety features at a wide range of operating temperatures. However, the Li-SOCl 2 battery system suffers from poor reversibility due to the sluggish kinetics of SOCl 2 reduction during discharging and the oxidation of the insulating discharge products during charging. To achieve a high-power rechargeable Li-SOCl 2 battery, herein we introduce the molecular catalyst I 2 into the electrolyte to tailor the charging and discharging reaction pathways. The as-assembled rechargeable cell exhibits superior power density, sustaining an ultrahigh current density of 100 mA cm −2 during discharging and delivering a reversible capacity of 1 mAh cm −2 for 200 cycles at a current density of 2 mA cm −2 and 6 mAh cm −2 for 50 cycles at a current density of 5 mA cm −2 . Our results reveal the molecular catalystmediated reaction mechanisms that fundamentally alter the rate-determining steps of discharging and charging in Li-SOCl 2 batteries and highlight the viability of transforming a primary high-energy battery into a high-power rechargeable system, which has great potential to meet the ever-increasing demand of energy-storage systems.

The Impact of Temperature on the Performance and Reliability of Li/SOCl2 Batteries

“…The EIS curves under this condition are represented by the blue curves in Figure 14a-c. When discharged with a 750 Ω resistance at a temperature of 25 • C, the high current breaks through the passivation layer attached to the Li metal negative electrode, forming holes that facilitate charge transfer through the passivation layer [20]. The damaged passivation layer exposes a larger area of the Li metal negative electrode to the electrolyte, reducing the charge transfer resistance on the Li metal surface.…”

Entropy Engineering toward Positive Temperature Coefficient and Large Voltage in High-Temperature Zinc-Ion Batteries

“…Batteries are essential for energy storage, widely utilized in devices ranging from automobiles to phones. − However, traditional batteries often fall short in meeting comprehensive demands, particularly in high-temperature performance. − Among various alternatives, aqueous zinc-ion batteries (AZIB) stand out due to their safety − and environmental benefits. − However, the zinc-ion batteries face voltage degradation at higher temperatures owing to increased entropy at the anode during discharge, as evidenced in NiHCF||ZnNH 3 , CuHCFe||Zn, and CF||Zn batteries (Figure ), demonstrating negative temperature coefficients of voltage (α = ∂ V /∂ T ) of −1.580, −0.980, and −2.47 mV·K –1 , respectively. , This voltage degradation hinders the zinc-ion batteries’ commercial viability. , …”

Enrichment of Chlorine in Porous Organic Nanocages for High-Performance Rechargeable Lithium–Chlorine Batteries

“…Recently, there has been an urgent pursuit of high-energy-density battery systems due to the rapid growth of electric vehicles and electronic products. − Rechargeable Li–Cl 2 batteries gradually attract people’s attention owing to their high energy density. − This kind of battery mainly consists of a Li/Li + negative electrode, a Cl – /Cl 2 positive electrode, and a SOCl 2 -based electrolyte, which could deliver a high discharge voltage of ∼3.5 V. However, cycling a Li–Cl 2 cell at a high specific capacity is still challenging, which restricts the energy density of the Li–Cl 2 battery. An important reason causing the failure of the Li–Cl 2 cell at a high cycling capacity is the insufficient supply of Cl 2 to the electrochemical reaction due to the weak interaction between cathode materials and Cl 2 molecules.…”