Liu Wen, Jiang Jianbing, Yang Ke R, Mi Yingying, Kumaravadivel Piranavan, Zhong Yiren, Fan Qi, Weng Zhe, Wu Zishan, Cha Judy J, Zhou Henghui, Batista Victor S, Brudvig Gary W, Wang Hailiang
Department of Chemistry and Energy Sciences Institute, Yale University, West Haven, CT 06516.
College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.
Proc Natl Acad Sci U S A. 2017 Apr 4;114(14):3578-3583. doi: 10.1073/pnas.1620809114. Epub 2017 Mar 20.
Lithium-sulfur batteries (Li-S batteries) have attracted intense interest because of their high specific capacity and low cost, although they are still hindered by severe capacity loss upon cycling caused by the soluble lithium polysulfide intermediates. Although many structure innovations at the material and device levels have been explored for the ultimate goal of realizing long cycle life of Li-S batteries, it remains a major challenge to achieve stable cycling while avoiding energy and power density compromises caused by the introduction of significant dead weight/volume and increased electrochemical resistance. Here we introduce an ultrathin composite film consisting of naphthalimide-functionalized poly(amidoamine) dendrimers and graphene oxide nanosheets as a cycling stabilizer. Combining the dendrimer structure that can confine polysulfide intermediates chemically and physically together with the graphene oxide that renders the film robust and thin (<1% of the thickness of the active sulfur layer), the composite film is designed to enable stable cycling of sulfur cathodes without compromising the energy and power densities. Our sulfur electrodes coated with the composite film exhibit very good cycling stability, together with high sulfur content, large areal capacity, and improved power rate.
锂硫电池(Li-S电池)因其高比容量和低成本而备受关注,尽管可溶的多硫化锂中间体导致其在循环过程中严重的容量损失,仍然阻碍了该电池的发展。尽管为了实现Li-S电池的长循环寿命这一最终目标,人们在材料和器件层面探索了许多结构创新,但在避免因引入大量无效重量/体积和增加电化学电阻而导致能量和功率密度受损的同时,实现稳定循环仍然是一项重大挑战。在此,我们引入了一种由萘二甲酰亚胺功能化的聚(酰胺胺)树枝状大分子和氧化石墨烯纳米片组成的超薄复合膜作为循环稳定剂。该复合膜结合了能够在化学和物理上限制多硫化物中间体的树枝状大分子结构以及使薄膜坚固且超薄(活性硫层厚度的<1%)的氧化石墨烯,旨在实现硫阴极的稳定循环,同时不损害能量和功率密度。涂覆有该复合膜的硫电极表现出非常好的循环稳定性,同时具有高硫含量、大面容量和改善的功率速率。