Millisecond lattice gasification for high-density CO 2 - and O 2 -sieving nanopores in single-layer graphene

• Published in: Science advances 2021-02, Vol.7 (9)
• Main Authors: Huang, Shiqi, Li, Shaoxian, Villalobos, Luis Francisco, Dakhchoune, Mostapha, Micari, Marina, Babu, Deepu J, Vahdat, Mohammad Tohidi, Mensi, Mounir, Oveisi, Emad, Agrawal, Kumar Varoon
• Format: Article
• Language: English
• ISSN: 2375-2548; 2375-2548
• DOI: 10.1126/sciadv.abf0116

Etching single-layer graphene to incorporate a high pore density with sub-angstrom precision in molecular differentiation is critical to realize the promising high-flux separation of similar-sized gas molecules, e.g., CO from N However, rapid etching kinetics needed to achieve the high pore density is challenging to control for such precision. Here, we report a millisecond carbon gasification chemistry incorporating high density (>10 cm ) of functional oxygen clusters that then evolve in CO -sieving vacancy defects under controlled and predictable gasification conditions. A statistical distribution of nanopore lattice isomers is observed, in good agreement with the theoretical solution to the isomer cataloging problem. The gasification technique is scalable, and a centimeter-scale membrane is demonstrated. Last, molecular cutoff could be adjusted by 0.1 Å by in situ expansion of the vacancy defects in an O atmosphere. Large CO and O permeances (>10,000 and 1000 GPU, respectively) are demonstrated accompanying attractive CO /N and O /N selectivities.