The three-dimensional (3D) macroscopic assembly of tailored porous architectures built of graphene derivatives or other two-dimensional (2D) materials has attracted great attention in both academia and industry. The reason being that such 3D assemblies with controlled morphology can provide ultra-large accessible surface areas and interconnected networks, as well as preventing the undesirable re-stacking phenomena of 2D materials. Herein, we review the synthetic routes and formation mechanism of bulk gel and interface mediated 3D architectures made of diverse 2D materials encompassing both graphene derivatives and non-graphene 2D materials. We also suggest universal strategies that can provide useful insight into application-oriented architecture design. The gelation mechanism is explained in detail; it involves controlled destabilization of the suspension involving a delicate balance between attractive and repulsive interactions. Further, interface mediated self-assembly processes between liquid-solid, liquid-liquid, liquid-gas, and ice-water phases are discussed with a view to tailoring 3D layered and interconnected morphologies. Finally, we highlight the demand for future applications of 2D material-based 3D macroporous architectures. Despite recent progress, more precise control strategies for tuning surface area, pore size distribution, orientation/interconnectivity of pores, density of architectures, and mechanical stability, remain as key scientific and technological barriers that must be addressed to enable practical applications. Further, an important frontier area for future research will involve multilateral hybridization, involving diverse combinations of materials, morphologies, and assembly methods This will provide researchers a multi-dimensional toolbox to access hitherto unavailable properties of 2D material-based 3D architectures for a whole host of applications.

中文翻译：

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二维材料构建的三维大孔结构的自组装和形态控制

由石墨烯衍生物或其他二维（2D）材料制成的定制多孔结构的三维（3D）宏观组装在学术界和工业界都引起了极大的关注。原因是这种具有受控形态的3D组件可以提供超大的可访问表面积和相互连接的网络，并可以防止2D材料的不良重新堆叠现象。本文中，我们回顾了由各种2D材料（包括石墨烯衍生物和非石墨烯2D材料）制成的块状凝胶和界面介导的3D体系结构的合成途径和形成机理。我们还建议了通用策略，这些策略可以对面向应用程序的体系结构设计提供有用的见解。详细说明了胶凝机理。它涉及悬浮液的受控失稳，包括吸引作用和排斥作用之间的微妙平衡。此外，为了调整3D分层和相互连接的形态，还讨论了液-固，液-液，液-气和冰-水相之间的界面介导的自组装过程。最后，我们强调了对基于2D材质的3D大孔结构未来应用的需求。尽管取得了最新进展，但用于调整表面积，孔径分布，孔的方向/互连性，结构的密度和机械稳定性的更精确的控制策略仍然是为实现实际应用而必须解决的关键科学技术障碍。此外，未来研究的重要前沿领域将涉及多边杂交，