TY - JOUR
T1 - Fabrication, Pressure Testing, and Nanopore Formation of Single-Layer Graphene Membranes
AU - Agrawal, Kumar Varoon
AU - Benck, Jesse D.
AU - Yuan, Zhe
AU - Misra, Rahul Prasanna
AU - Govind Rajan, Ananth
AU - Eatmon, Yannick
AU - Kale, Suneet
AU - Chu, Ximo S.
AU - Li, Duo O.
AU - Gong, Chuncheng
AU - Warner, Jamie
AU - Wang, Qing
AU - Blankschtein, Daniel
AU - Strano, Michael S.
N1 - Funding Information:
This work was supported in part by the U.S. Army Research Laboratory and the U.S. Army Research Office through the Institute for Soldier Nanotechnologies, under contract number W911NF-13-D-0001. Q.H.W. acknowledges support from Arizona State University startup funds.
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/7/6
Y1 - 2017/7/6
N2 - Single-layer graphene (SLG) membranes have great promise as ultrahigh flux, high selectivity membranes for gas mixture separations due to their single atom thickness. It remains a central question whether SLG membranes of a requisite area can exist under an imposed pressure drop and temperatures needed for industrial gas separation. An additional challenge is the development of techniques to perforate or otherwise control the porosity in graphene membranes to impart molecularly sized pores, the size regime predicted to produce high gas separation factors. Herein, we report fabrication, pressure testing, temperature cycling, and gas permeance measurements through free-standing, low defect density SLG membranes. Our measurements demonstrate the remarkable chemical and mechanical stability of these 5 μm diameter suspended SLG membranes, which remain intact over weeks of testing at pressure differentials of >0.5 bar, repeated temperature cycling from 25 to 200 °C, and exposure to 15 mol % ozone for up to 3 min. These membranes act as molecularly impermeable barriers, with very low or near negligible background permeance. We also demonstrate a 1077 °C temperature O2 etching technique to create nanopores on the order of ∼1 nm diameter as imaged by scanning tunneling microscopy, although transport through such pores has not yet been successfully measured. Overall, these results represent an important advancement that will enable graphene gas separation membranes to be fabricated, tested, and modified in situ while maintaining remarkable mechanical and thermal stability.
AB - Single-layer graphene (SLG) membranes have great promise as ultrahigh flux, high selectivity membranes for gas mixture separations due to their single atom thickness. It remains a central question whether SLG membranes of a requisite area can exist under an imposed pressure drop and temperatures needed for industrial gas separation. An additional challenge is the development of techniques to perforate or otherwise control the porosity in graphene membranes to impart molecularly sized pores, the size regime predicted to produce high gas separation factors. Herein, we report fabrication, pressure testing, temperature cycling, and gas permeance measurements through free-standing, low defect density SLG membranes. Our measurements demonstrate the remarkable chemical and mechanical stability of these 5 μm diameter suspended SLG membranes, which remain intact over weeks of testing at pressure differentials of >0.5 bar, repeated temperature cycling from 25 to 200 °C, and exposure to 15 mol % ozone for up to 3 min. These membranes act as molecularly impermeable barriers, with very low or near negligible background permeance. We also demonstrate a 1077 °C temperature O2 etching technique to create nanopores on the order of ∼1 nm diameter as imaged by scanning tunneling microscopy, although transport through such pores has not yet been successfully measured. Overall, these results represent an important advancement that will enable graphene gas separation membranes to be fabricated, tested, and modified in situ while maintaining remarkable mechanical and thermal stability.
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U2 - 10.1021/acs.jpcc.7b01796
DO - 10.1021/acs.jpcc.7b01796
M3 - Article
AN - SCOPUS:85024477207
SN - 1932-7447
VL - 121
SP - 14312
EP - 14321
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 26
ER -