2D heterostructures offer a great opportunity in seeking high-performing energy storage materials; however, performance ceiling exists, limited by their van-der-Waals (vdW) interactions. Here, we explore a novel 2D, amorphous MoO_3−x (aMoO_3−x) on Ti₃C₂-MXene, non-vdW heterostructure via a facile synthesis route. Density functional theory computations suggest that the non-vdW heterostructure can strongly stabilize aMoO_3−x while maintaining electrical conductivity at a high level. Facile 2D Li-ion diffusion can then be achieved in the restacked 2D non-vdW heterostructures due to the weakened interactions between two defective MoO_3−x layers, leading to a capacitor-like interlayer diffusion reaching a large capacity of 426 C g⁻¹ on the surface of the amorphous layer and a diffusion-controlled intralayer diffusion of 546 C g⁻¹ within the amorphous layer. These characteristics optimize Li-ion storage kinetics while achieving full capacities of amorphous materials with high stability. This work might offer a feasible platform of 2D non-vdW heterostructures for boosting and understanding Li-ion storage performance.

2D异质结构为寻求高性能储能材料提供了巨大的机会。但是，存在性能上限，这受它们的van-der-Waals（vdW）交互作用的限制。在这里，我们通过一种简便的合成途径探索了在Ti ₃ C ₂ -MXene的非vdW异质结构上的新型2D，非晶MoO _3-x（aMoO _3-x）。密度泛函理论计算表明，非vdW异质结构可以在保持高电导率的同时，使aMoO _3-x稳定。由于两个有缺陷的MoO _3-x之间的相互作用减弱，因此可以在重新堆叠的2D非vdW异质结构中实现便捷的2D锂离子扩散层，导致电容器状层间扩散在非晶层的表面上达到426 C g ^-1的大容量，并且在非晶层内扩散控制的546 C g ^-1的层内扩散。这些特性优化了锂离子的存储动力学，同时实现了具有高稳定性的非晶态材料的全部容量。这项工作可能会提供2D非vdW异质结构的可行平台，以提高和了解锂离子存储性能。