Sulfur and polysulfides play important roles on the environment and energy storage systems, especially in the recent hot area of high energy density of lithium−sulfur (Li− S) batteries. However, the further development of Li−S battery is still retarded by the lack of complete mechanistic understanding of the sulfur redox process. Herein we introduce a conductive Lewis base matrix which has the ability to enhance the battery performance of Li−S battery, via the understanding of the complicated sulfur redox chemistry on the electrolyte/ carbon interface by a combined in operando Raman spectroscopy and density functional theory (DFT) method. The higher polysulfides, Li 2 S 8 , is found to be missing during the whole redox route, whereas the charging process of Li−S battery is ended up with the Li 2 S 6 . DFT calculations reveal that Li 2 S 8 accepts electrons more readily than S 8 and Li 2 S 6 so that it is thermodynamically and kinetically unstable. Meanwhile, the poor adsorption behavior of Li 2 S n on carbon surface further prevents the oxidization of Li 2 S n back to S 8 upon charging. Periodic DFT calculations show that the N-doped carbon surface can serve as conductive Lewis base "catalyst" matrix to enhance the adsorption energy of Li 2 S n (n = 4−8). This approach allows the higher Li 2 S n to be further oxidized into S 8 , which is also confirmed by in operando Raman spectroscopy. By recovering the missing link of Li 2 S 8 in the whole redox route, a significant improvement of the S utilization and cycle stability even at a high sulfur loading (70%, m/m) in the composite on a simple super P carbon.
Perovskite
solar cells are strong competitors for silicon-based
ones, but suffer from poor long-term stability, for which the intrinsic
stability of perovskite materials is of primary concern. Herein, we
prepared a series of well-defined cesium-containing mixed cation and
mixed halide perovskite single-crystal alloys, which enabled systematic
investigations on their structural stabilities against light, heat,
water, and oxygen. Two potential phase separation processes are evidenced
for the alloys as the cesium content increases to 10% and/or bromide
to 15%. Eventually, a highly stable new composition, (FAPbI3)0.9(MAPbBr3)0.05(CsPbBr3)0.05, emerges with a carrier lifetime of 16 μs.
It remains stable during at least 10 000 h water–oxygen
and 1000 h light stability tests, which is very promising for long-term
stable devices with high efficiency. The mechanism for the enhanced
stability is elucidated through detailed single-crystal structure
analysis. Our work provides a single-crystal-based paradigm for stability
investigation, leading to the discovery of stable new perovskite materials.
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