Artificial heterostructures with structural advancements and customizable electronic interfaces are fundamental for achieving high-performance lithium-ion batteries (LIBs). Here, a design idea for a covalently bonded lateral/vertical black phosphorus (BP)-graphdiyne oxide (GDYO) heterostructure achieved through a facile ball-milling approach, is designed. Lateral heterogeneity is realized by the sp²-hybridized mode P-C bonds, which connect the phosphorus atoms at the edges of BP with the carbon atoms of the terminal acetylene in GDYO. The vertical connection of the heterojunction of BP and GDYO is connected by P-O-C bond. Experimental and theoretical studies demonstrate that BP-GDYO incorporates interfacial and structural engineering features, including built-in electric fields, chemical bond interactions, and maximized nanospace confinement effects. Therefore, BP-GDYO exhibits improved electrochemical kinetics and enhanced structural stability. Moreover, through ex- and in-situ studies, the lithiation mechanism of BP-GDYO, highlighting that the introduction of GDYO inhibits the shuttle/dissolution effect of phosphorus intermediates, hinders volume expansion, provides more reactive sites, and ultimately promotes reversible lithium storage, is clarified. The BP-GDYO anode exhibits lithium storage performance with high-rate capacity and long-cycle stability (602.6 mAh g⁻¹ after 1 000 cycles at 2.0 A g⁻¹). The proposed interfacial and structural engineering is universal and represents a conceptual advance in building high-performance LIBs electrode.

中文翻译：

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用于锂存储的受控生长横向/垂直异质结构界面

具有结构进步和可定制电子接口的人造异质结构是实现高性能锂离子电池（LIB）的基础。在这里，设计了一种通过简单的球磨方法实现的共价键合的横向/垂直黑磷（BP）-氧化石墨二炔（GDYO）异质结构。横向异质性是通过sp ²杂化模式PC键实现的，该键将BP边缘的磷原子与GDYO中末端乙炔的碳原子连接起来。 BP和GDYO异质结的垂直连接通过POC键连接。实验和理论研究表明，BP-GDYO 结合了界面和结构工程特征，包括内置电场、化学键相互作用和最大化纳米空间限制效应。因此，BP-GDYO表现出改进的电化学动力学和增强的结构稳定性。此外，通过离位和原位研究，揭示了BP-GDYO的锂化机理，强调GDYO的引入抑制了磷中间体的穿梭/溶解效应，阻碍了体积膨胀，提供了更多的反应位点，最终促进了可逆的锂存储，已澄清。 BP-GDYO负极表现出具有高倍率容量和长循环稳定性的锂存储性能（在2.0 A g ^-1下循环1000次后为602.6 mAh g ^-1）。所提出的界面和结构工程是通用的，代表了构建高性能锂离子电池电极的概念进步。