Ashirov, T; Yazaydin, AO; Coskun, A; (2022) Tuning the Transport Properties of Gases in Porous Graphene Membranes with Controlled Pore Size and Thickness. Advanced Materials , 34 (5) , Article 2106785. 10.1002/adma.202106785.

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Abstract

Porous graphene membranes emerged as promising alternatives for gas separation applications due to their atomic thickness enabling ultra-high permeance, but suffer from low gas selectivity. Whereas decreasing the pore size below 3 nm is expected to increase the gas selectivity due to molecular sieving, it is rather challenging to generate large number of uniform small pores on the graphene surface. Here, we introduce a pore narrowing approach via gold deposition onto porous graphene surface to tune the pore size and thickness of the membrane to achieve large number of small pores. Through our systematic approach, we determined the ideal combination as pore size below 3 nm obtained at the thickness of 100 nm to attain high selectivity and high permeance. The resulting membrane showed a H2 /CO2 separation factor of 31.3 at H2 permeance of 2.23 × 105 GPU (1 GPU = 3.35 × 10-10  mol s-1 m-2 Pa-1 ), which is the highest value reported to date in the 105 GPU permeance range. This result is explained by comparing the predicted binding energies of gas molecules with the Au surface, -5.3 versus -21 kJ mol-1 for H2 and CO2 , respectively, increased surface-gas interactions and molecular sieving effect with decreasing pore size. This article is protected by copyright. All rights reserved.

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