Layer-on-layer assembly of macroscopic 2D and 3D carbon nanomaterial architectures

There are major shortcomings in the assembly of carbon nanomaterials into higher order structures. Two- and three-dimensional structiues are required for many desirable applications of these materials. Present methods for 2D assembhes include challenges with regards to scalability, suitability for a large variety of substrates, mechanical stability, and/or biocompatibility. Very few strategies exist for fabrication of three-dimensional structures. We developed an easily scalable spray coating fabrication process for in situ chemical crosslinking of carbon nanomaterials to develop more robust, flexible, and biocompatible coatings/films. Furthermore, the process has been adapted to provide a layer-on-layer deposition of nanomaterials into three-dimensional structures. This work enables the fabrication of more robust carbon nanotube and graphene coatings by a facile, scalable, and flexible method. It also elucidates a potential enabling technology for all-carbon nanomaterial 3D printing.