Journal
ACS NANO
Volume 16, Issue 7, Pages 11102-11114Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c03788
Keywords
copper selenide; phase engineering; copper vacancies; lithium-sulfur battery; lithium polysulfide
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This study proposes a method of adding copper selenide nanoparticles to the cathode of lithium-sulfur batteries to trap soluble lithium polysulfides and accelerate the reaction kinetics. By adjusting the crystal phase and defect density of the copper selenide, the electronic structure, affinity toward lithium polysulfides, and electrical conductivity can be controlled, resulting in improved battery performance.
The shuttling of soluble lithium polysulfides (LiPS) and the sluggish Li-S conversion kinetics are two main barriers toward the practical application of lithium-sulfur batteries (LSBs). Herein, we propose the addition of copper selenide nanoparticles at the cathode to trap LiPS and accelerate the Li-S reaction kinetics. Using both computational and experimental results, we demonstrate the crystal phase and concentration of copper vacancies to control the electronic structure of the copper selenide, its affinity toward LiPS chemisorption, and its electrical conductivity. The adjustment of the defect density also allows for tuning the electrochemically active sites for the catalytic conversion of polysulfide. The optimized S/Cu1.8Se cathode efficiently promotes and stabilizes the sulfur electrochemistry, thus improving significantly the LSB performance, including an outstanding cyclability over 1000 cycles at 3 C with a capacity fading rate of just 0.029% per cycle, a superb rate capability up to 5 C, and a high areal capacity of 6.07 mAh cm(-2) under high sulfur loading. Overall, the present work proposes a crystal phase and defect engineering strategy toward fast and durable sulfur electrochemistry, demonstrating great potential in developing practical LSBs.
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