Direct coating of Si on an elastic carbon nanotube (CNT) network effectively addresses the rapid capacity fading of the Si anode. However, this strategy is hindered by the low Si tap density (Si < 50 nm) since sufficient void space has to be left for accommodating the Si volume change. Also, the mechanical properties of the CNT network as the elastic buffer matrix degrade significantly caused by side reactions of CNT with electrolyte. This work presents a freestanding paper-like anode consisting of a symmetrical sandwich-structured SiN/Si/SiN composite grown on CNT paper. This anode works well (∼259 μA h cm-2 under the current rate of 0.6C after 350 cycles, with a capacity retention of 73.8%) even when the CNT is filled by the composite without void space left for accommodating volume expansion. This is mainly due to the following synergistic effects: on one hand, the stress-compensation phenomenon in the symmetrical sandwich-structured composite balances the volume change-induced stress and thus the composite has a robust mechanical stability with an intact morphology during cycling. On the other hand, the intact composite avoids reaction of CNT with the electrolyte and thus the CNT retains excellent mechanical properties and serves well as the elastic buffer matrix. These two sides interact with each other, enabling the high anode performance.
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