A High‐Energy Long‐Cycling Solid‐State Lithium‐Metal Battery Operating at High Temperatures

Abstract

High‐energy rechargeable lithium‐ion batteries, especially solid‐state lithium metal batteries, are increasingly required to operate at elevated temperatures in addition to pursuing operation at low temperatures. However, the notorious chemical and electrochemical reactions at the interface between the Li‐anode and solid state electrolyte (SSE) make these batteries lose almost all of their capacity and power at elevated temperatures. Here, a safe and long‐cycle‐life solid‐state Li–CO2 battery operating at elevated temperatures by constructing a stable and high ionic conductive molten salts interface (MSI) is reported. The MSI can effectively improve the interface contact and suppress interface reactions and the thermal runaway between Li‐anode and Li1.5Al0.5Ge1.5P3O12 (LAGP)‐electrolyte even at high temperatures, thus enabling an ultra‐low interface impedance (≈15 Ω) and discharge/charge overpotential (≈15 mV) for high temperature symmetric battery. In addition, the MSI‐coated LAGP‐electrolyte shows an ultra‐flat and continuous surface that enables a homogeneous Li tripping/plating during cycles. As a result, the Li symmetric battery shows superior cycling stability over 600 h at 0.1 mA cm−2 at 150 °C. The assembled solid‐state Li–CO2 battery using Ru catalysts shows outstanding cycle stability over 980 cycles at 150 °C, with a capacity limitation of 500 mAhg–1 at 500 mA g−1.

Solvent-Free and Long-Cycling Garnet-Based Lithium-Metal Batteries

“…As we know, commercial lithium batteries are expected to be operated at mild temperatures of 45−60 °C as well as even tough temperatures of 80−100 °C for desert area, medical sterilization, oil/gas explorations and space application. 53 Hence, the Li||LFP cells were tested at 45 °C and 80/100 °C as well to inspect the melting point and thermal stability (Figure 2f). The cells could output the capacity up to 153.3 mAh g −1 initially and was able to retain 83.8% of the capacity after 200 cycles at 0.5 C, compared to the similar battery performance with a liquid electrolyte at 45 °C (Figure 2f and Figure S13).…”

“…For the counterpart with a liquid electrolyte, the batteries could indeed work stably at room temperature (Figure S13) but suffer from serious capacity decay at 60 °C (Figure d) because of its inferior thermal stability. As we know, commercial lithium batteries are expected to be operated at mild temperatures of 45–60 °C as well as even tough temperatures of 80–100 °C for desert area, medical sterilization, oil/gas explorations and space application . Hence, the Li||LFP cells were tested at 45 °C and 80/100 °C as well to inspect the melting point and thermal stability (Figure f).…”

Gallium Nitride Based Electrode for High‐Temperature Supercapacitors

“…[ 4 ] Especially in high‐temperature environments, such as the engine cover of hybrid electric vehicles can exceed 140 °C and the locate temperature of specific tasks (subsurface exploration, medical rescue, and military) may be more than 250 °C. [ 5 ] SCs have become mainstream applications since most electrolytes in commercial organic batteries with boiling points below 80 °C lead to the instability of devices. [ 6 ] Therefore, it is necessary to develop reliable, safe, and prominent performance SCs that operate under high‐temperature conditions.…”

Fast Ion Conduction Nanofiber Matrix Composite Electrolyte for Dendrite‐Free Solid‐State Sodium‐Ion Batteries with Wide Temperature Operation

“…Scalable electrospinning technology has been developed for fabricating nanofibrous separators in our previous work, [ 31 ] which provides the technical support for large‐scale ceramic nanofibrous membrane incorporation into polymer electrolytes to achieve thermostability, which is promising for use in the military or medical field. [ 32 ]…”

“…Scalable electrospinning technology has been developed for fabricating nanofibrous separators in our previous work, [31] which provides the technical support for large-scale ceramic nanofibrous membrane incorporation into polymer electrolytes to achieve thermostability, which is promising for use in the military or medical field. [32] In addition, sodium dendrite is also a challenge, restricting the practical application of SIBs. [33] For throttling the alkali dendrites, it is critical to control the electron-ion transfer process at the interface of the anode and electrolyte.…”