Lithium (Li) hosts, which can electrochemically accommodate Li in preformed pores of three-dimensional frameworks, have been investigated as an advanced electrode architecture for high-energy-density Li-metal batteries. However, most of the previous studies on Li hosts utilized electrochemically inert materials for their framework constituents, resulting in undesired loss of gravimetric/volumetric energy densities of the resulting batteries. Here, we present an electroactive Li host based on a microgrid-patterned Si electrode (denoted as the MPS host). The MPS host is fabricated using a microscale direct ink writing technique. The lithiophilicity, electronic conductivity, and porous structure of the MPS host are customized to ensure the preferential direction of Li–ion flux and electron conduction into the ordered pore space, while providing the redox capacity. The resulting MPS host enables stepwise sequential Si lithiation/delithiation (from the Si in the microgrid frameworks) and Li plating/stripping (inside the pore space between the microgrids) reactions, verifying its unique behavior as an electroactive Li host. In addition, a full cell assembled with the MPS host and the LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathode (areal capacity = 3.8 mAh cm⁻²) exhibits high cell energy densities (644 Wh kg_cell⁻¹/1538 Wh L_cell⁻¹) and reliable cyclability.

中文翻译：

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微网格图案的硅电极作为电活性锂主体

锂 (Li) 主体可以电化学地将锂容纳在三维框架的预制孔中，已被研究为用于高能量密度锂金属电池的先进电极结构。然而，之前关于锂主体的大多数研究都使用电化学惰性材料作为其框架成分，导致所得电池的重量/体积能量密度不希望有损失。在这里，我们提出了一种基于微网格图案 Si 电极（称为 MPS 主体）的电活性锂主体。MPS 主机是使用微型直接墨水书写技术制造的。MPS主体的亲锂性、电子导电性和多孔结构是定制的，以确保锂离子通量和电子传导到有序孔隙空间的优先方向，同时提供氧化还原能力。由此产生的 MPS 主体能够实现逐步顺序的硅锂化/脱锂（来自微电网框架中的硅）和锂电镀/剥离（在微电网之间的孔隙空间内）反应，验证了其作为电活性锂主体的独特行为。此外，由 MPS 主机和 LiNi 组装的全电池_0.8 Co _0.1 Mn _0.1 O ₂ (NCM811)正极（面积容量= 3.8 mAh cm ^-2）表现出高电池能量密度（644 Wh kg _cell ^-1 /1538 Wh L _cell ^-1）和可靠的可循环性。