Nacre-like MXene/polyacrylic acid layer-by-layer multilayers as hydrogen gas barriers

Auh, Y. H.*; Neal, N. N.*; Arole, K.*; Regis, N. A.*; Nguyen, T.*; Ogawa, Shuichi*; Tsuda, Yasutaka   ; Yoshigoe, Akitaka ; Radovic, M.*; Green, M. J.*; Yamaguchi, Hisato*; Lutkenhaus, J. L.*

MXenes are a promising class of 2D nanomaterials and are of particular interest for gas barrier application. However, MXene nanosheets naturally bear a negative charge, which prevents assembly with negatively charged polymers, such as polyacrylic acid (PAA), into gas barrier coatings. Here, we present MXene- and PAA-based layer-by-layer (MXene/PAA LbL) multilayers formed by leveraging hydrogen bonding interactions. When assembled in acidic conditions, MXene/PAA LbL films exhibit conformal, pin-hole free, nacre-like structures. The MXene/PAA LbL films yield high blocking capability and low permeability (0.140.01 cc mm m day MPa) for hydrogen gas. These nacre-like structures are also electronically conductive (up to 37030 S cm). Specifically, the reversible deconstruction of these films under basic conditions is experimentally verified. This study shows that hydrogen bonding interactions can be leveraged to form MXene LbL multilayers as gas barriers, electronically conducive coatings, and deconstructable thin films via pH control.