Highly elastic binders integrating polyrotaxanes for silicon microparticle anodes in lithium ion batteries

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Science  21 Jul 2017:
Vol. 357, Issue 6348, pp. 279-283
DOI: 10.1126/science.aal4373

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A stretchy binder protects the silicon

A challenge in using silicon particles for lithium batteries is that the large volume changes during charge-discharge cycling cause the particles to fracture, which builds up an insulating interface layer. Choi et al. show that traditional binder materials used to cushion the silicon particles can be improved by adding small amounts of polyrotaxanes (see the Perspective by Ryu and Park). The molecules consist of multiple rings that are strung along a linear segment and stoppered at each end. Some of the rings are anchored to the polymer binder, whereas others float freely, yielding a highly mobile but connected network that anchors the binder, and thus the silicon particles, together.

Science, this issue p. 279; see also p. 250


Lithium-ion batteries with ever-increasing energy densities are needed for batteries for advanced devices and all-electric vehicles. Silicon has been highlighted as a promising anode material because of its superior specific capacity. During repeated charge-discharge cycles, silicon undergoes huge volume changes. This limits cycle life via particle pulverization and an unstable electrode-electrolyte interface, especially when the particle sizes are in the micrometer range. We show that the incorporation of 5 weight % polyrotaxane to conventional polyacrylic acid binder imparts extraordinary elasticity to the polymer network originating from the ring sliding motion of polyrotaxane. This binder combination keeps even pulverized silicon particles coalesced without disintegration, enabling stable cycle life for silicon microparticle anodes at commercial-level areal capacities.

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