The Li–O₂ battery is one of the most captivating energy storage forms due to its extraordinarily high energy density and the readily its the ready availability of oxygen. However, significant challenges lie ahead on both the anode and cathode sides before the technology can be finally deployed to benefit human life. Herein, a two‐birds‐one‐stone tactic is implemented to fabricate high‐performance and flexible Li–O₂ batteries utilizing only one structural backbone composed of graphene oxide aerogel embedding hollow NiCo₂O₄ microspheres for both the anode and cathode. While the composite Li anode fabricated through lithium infusion exhibits an ultrahigh capacity of 3398.4 mAh g⁻¹ and significantly inhibits dendrite growth and volume expansion, the freestanding oxygen cathode demonstrates great capability in promoting energy efficiency by catalyzing reversible Li₂O₂ formation. When coupled together, the resultant Li–O₂ batteries manifest a superb long‐term cycling stability with highly reversible discharge/charge for more than 400 cycles, apart from the remarkable mechanical deformability demonstrated by flexible pouch cells. By employing a full spectrum of ex situ and operando spectroscopic and microscopic tools, mechanistic insights into the remarkable Li–O₂ performance are given.

中文翻译：

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基于全石墨烯骨架的高性能Li-O2电池

Li–O ₂电池是最吸引人的能量存储形式之一，因为它具有极高的能量密度和容易获得的氧气。然而，在最终使这项技术造福人类生活之前，阳极和阴极方面都面临着巨大的挑战。本文采用两鸟一石策略来制造高性能且灵活的Li-O ₂电池，该电池仅使用一个由氧化石墨烯气凝胶嵌入空心NiCo ₂ O ₄微球构成的结构主干作为阳极和阴极。通过锂注入制备的复合锂阳极表现出3398.4 mAh g ^-1的超高容量独立的氧阴极通过催化可逆的Li ₂ O ₂形成，具有显着的提高能量效率的能力，并且显着抑制枝晶的生长和体积膨胀。结合在一起后，所得的Li–O ₂电池具有出色的长期循环稳定性，并且在超过400个循环中具有高度可逆的放电/充电能力，此外还有柔性袋式电池具有显着的机械变形能力。通过使用全光谱的异位，操作光谱和显微工具，可以对显着的Li-O ₂性能进行机械分析。