Journal
NANO-MICRO LETTERS
Volume 14, Issue 1, Pages -Publisher
SHANGHAI JIAO TONG UNIV PRESS
DOI: 10.1007/s40820-021-00769-2
Keywords
High-index faceted; Fe2O3 nanocrystals; Unsaturated coordinated; Lithium-sulfur batteries; Electrocatalysis
Funding
- Shanghai Jiao Tong University
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The surface structure of crystal-line materials was precisely regulated to improve the catalytic activity of lithium polysulfides, leading to the development of high-index faceted iron oxide nanocrystals as highly efficient bifunctional electrocatalysts for lithium-sulfur batteries. The high-index Fe2O3 crystal facets with unsaturated coordinated Fe sites exhibited strong adsorption capacity for polysulfides and high catalytic activity for the redox transformation, resulting in enhanced electrochemical performance and cycling stability of Li-S batteries.
Precisely regulating of the surface structure of crystal- line materials to improve their catalytic activity for lithium polysulfides is urgently needed for high-performance lithium-sulfur (Li-S) batteries. Herein, high-index faceted iron oxide (Fe2O3) nanocrystals anchored on reduced graphene oxide are developed as highly efficient bifunctional electrocatalysts, effectively improving the electrochemical performance of Li-S batteries. The theoretical and experimental results all indicate that high-index Fe2O3 crystal facets with abundant unsaturated coordinated Fe sites not only have strong adsorption capacity to anchor polysulfides but also have high catalytic activity to facilitate the redox transformation of polysulfides and reduce the decomposition energy barrier of Li2S. The Li-S batteries with these bifunctional electrocatalysts exhibit high initial capacity of 1521 mAh g(-1) at 0.1 C and excellent cycling performance with a low capacity fading of 0.025% per cycle during 1600 cycles at 2 C. Even with a high sulfur loading of 9.41 mg cm(-2) , a remarkable areal capacity of 7.61 mAh cm(-2) was maintained after 85 cycles. This work provides a new strategy to improve the catalytic activity of nanocrystals through the crystal facet engineering, deepening the comprehending of facet-dependent activity of catalysts in Li-S chemistry, affording a novel perspective for the design of advanced sulfur electrodes.
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