Oxidation States Regulation of Cobalt Active Sites through Crystal Surface Engineering for Enhanced Polysulfide Conversion in Lithium-Sulfur Batteries.
Rujian XiaoDan LuoJiayi WangHan LuHeng MaEser Metin AkinogluMingliang JinXin WangYongguang ZhangZhongwei ChenPublished in: Advanced science (Weinheim, Baden-Wurttemberg, Germany) (2022)
In this work, unique Co 3 O 4 /N-doped reduced graphene oxide (Co 3 O 4 /N-rGO) composites as favorable sulfur immobilizers and promoters for lithium-sulfur (Li-S) batteries are developed. The prepared Co 3 O 4 nanopolyhedrons (Co 3 O 4 -NP) and Co 3 O 4 nanocubes mainly expose (112) and (001) surfaces, respectively, with different atomic configurations of Co 2+ /Co 3+ sites. Experiments and theoretical calculations confirm that the octahedral coordination Co 3+ (Co 3+ Oh ) sites with different oxidation states from tetrahedral coordination Co 2+ sites optimize the adsorption and catalytic conversion of lithium polysulfides. Specially, the Co 3 O 4 -NP crystals loaded on N-rGO expose (112) planes with ample Co 3+ Oh active sites, exhibiting stronger adsorbability and superior catalytic activity for polysulfides, thus inhibiting the shuttle effect. Therefore, the S@Co 3 O 4 -NP/N-rGO cathodes deliver excellent electrochemical properties, for example, stable cyclability at 1 C with a low capacity decay rate of 0.058% over 500 cycles, superb rate capability up to 3 C, and high areal capacity of 4.1 mAh cm -2 . This catalyst's design incorporating crystal surface engineering and oxidation state regulation strategies also provides new approaches for addressing the complicated issues of Li-S batteries.
Keyphrases
- reduced graphene oxide
- solid state
- gold nanoparticles
- visible light
- hydrogen peroxide
- drug delivery
- quantum dots
- ion batteries
- escherichia coli
- ionic liquid
- signaling pathway
- high resolution
- room temperature
- molecular dynamics simulations
- biofilm formation
- nitric oxide
- staphylococcus aureus
- mass spectrometry
- cystic fibrosis
- molecularly imprinted