Chae Sujong, Xu Yaobin, Yi Ran, Lim Hyung-Seok, Velickovic Dusan, Li Xiaolin, Li Qiuyan, Wang Chongmin, Zhang Ji-Guang
Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, 99354, USA.
Department of Industrial Chemistry, Pukyong National University, Busan, 48513, Republic of Korea.
Adv Mater. 2021 Oct;33(40):e2103095. doi: 10.1002/adma.202103095. Epub 2021 Aug 16.
Porous silicon (Si)/carbon nanocomposites have been extensively explored as a promising anode material for high-energy lithium (Li)-ion batteries (LIBs). However, shrinking of the pores and sintering of Si in the nanoporous structure during fabrication often diminishes the full benefits of nanoporous Si. Herein, a scalable method is reported to preserve the porous Si nanostructure by impregnating petroleum pitch inside of porous Si before high-temperature treatment. The resulting micrometer-sized Si/C composite maintains a desired porosity to accommodate large volume change and high conductivity to facilitate charge transfer. It also forms a stable surface coating that limits the penetration of electrolyte into nanoporous Si and minimizes the side reaction between electrolyte and Si during cycling and storage. A Si-based anode with 80% of pitch-derived carbon/nanoporous Si enables very stable cycling of a Si||Li(Ni0.5Co0.2Mn0.3)O (NMC532) battery (80% capacity retention after 450 cycles). It also leads to low swelling in both particle and electrode levels required for the next generation of high-energy LIBs. The process also can be used to preserve the porous structure of other nanoporous materials that need to be treated at high temperatures.
多孔硅(Si)/碳纳米复合材料作为一种有前景的高能锂离子电池(LIBs)负极材料已被广泛研究。然而,在制备过程中,纳米多孔结构中的孔隙收缩和硅的烧结常常削弱了纳米多孔硅的全部优势。在此,报道了一种可扩展的方法,即在高温处理之前将石油沥青浸渍到多孔硅内部,以保留多孔硅纳米结构。所得的微米级硅/碳复合材料保持了所需的孔隙率以适应大的体积变化,并具有高导电性以促进电荷转移。它还形成了稳定的表面涂层,限制了电解质渗透到纳米多孔硅中,并使循环和储存过程中电解质与硅之间的副反应最小化。具有80%沥青衍生碳/纳米多孔硅的硅基负极可使硅||锂(Ni0.5Co0.2Mn0.3)O(NMC532)电池实现非常稳定的循环(450次循环后容量保持率为80%)。它还导致下一代高能锂离子电池所需的颗粒和电极水平的低膨胀。该工艺还可用于保留其他需要高温处理的纳米多孔材料的多孔结构。