Selective proton permeation through the atomically thin lattice of graphene and other 2D materials offers newpossibilities for energy conversion/storage and novel separations. Practical applications necessitate scalable synthesisvia approaches such as chemical vapor deposition (CVD) that inevitably introduce sub-nanometer defects, grainboundaries and wrinkles, and understanding their influence on H+ transport and selectivity for large-area membranes isimperative but remains elusive. Using electrically-driven transport of protons and other ions through monolayer CVDgraphene we systematically deconstruct selective proton transport. Mitigation of large defects, wrinkles and tears viainterfacial polymerization results in selective proton permeation rates comparable to state-of-the-art proton exchangemembranes e.g. Nafion. Our work provides a new framework to assess H+ conductance and selectivity of large-area2D membranes for practical applications.

Deconstructing proton transport through atomically thin monolayer CVD graphene membranes

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ACS Fall 2022

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