TY - JOUR
T1 - Gas-sieving zeolitic membranes fabricated by condensation of precursor nanosheets
AU - Dakhchoune, Mostapha
AU - Villalobos, Luis Francisco
AU - Semino, Rocio
AU - Liu, Lingmei
AU - Rezaei, Mojtaba
AU - Schouwink, Pascal
AU - Avalos, Claudia Esther
AU - Baade, Paul
AU - Wood, Vanessa
AU - Han, Yu
AU - Ceriotti, Michele
AU - Agrawal, Kumar Varoon
N1 - Funding Information:
We thank our host institution, EPFL, for generous support. This work was primarily funded by the Swiss Competence Center for Energy Research: Efficiency of Industrial Processes (SCCER-EIP). A part of this work was funded by the Swiss National Science Foundation (Assistant Professor Energy Grant, grant no. PYAPP2-173645). The computational aspects of this work were supported by a grant from the Swiss National Supercomputing Centre (CSCS) under project ID s887. We acknowledge E. Oveisi for the helpful discussions on electron microscopy.
Publisher Copyright:
© 2020, The Author(s), under exclusive licence to Springer Nature Limited.
PY - 2021/3
Y1 - 2021/3
N2 - The synthesis of molecular-sieving zeolitic membranes by the assembly of building blocks, avoiding the hydrothermal treatment, is highly desired to improve reproducibility and scalability. Here we report exfoliation of the sodalite precursor RUB-15 into crystalline 0.8-nm-thick nanosheets, that host hydrogen-sieving six-membered rings (6-MRs) of SiO4 tetrahedra. Thin films, fabricated by the filtration of a suspension of exfoliated nanosheets, possess two transport pathways: 6-MR apertures and intersheet gaps. The latter were found to dominate the gas transport and yielded a molecular cutoff of 3.6 Å with a H2/N2 selectivity above 20. The gaps were successfully removed by the condensation of the terminal silanol groups of RUB-15 to yield H2/CO2 selectivities up to 100. The high selectivity was exclusively from the transport across 6-MR, which was confirmed by a good agreement between the experimentally determined apparent activation energy of H2 and that computed by ab initio calculations. The scalable fabrication and the attractive sieving performance at 250–300 °C make these membranes promising for precombustion carbon capture.
AB - The synthesis of molecular-sieving zeolitic membranes by the assembly of building blocks, avoiding the hydrothermal treatment, is highly desired to improve reproducibility and scalability. Here we report exfoliation of the sodalite precursor RUB-15 into crystalline 0.8-nm-thick nanosheets, that host hydrogen-sieving six-membered rings (6-MRs) of SiO4 tetrahedra. Thin films, fabricated by the filtration of a suspension of exfoliated nanosheets, possess two transport pathways: 6-MR apertures and intersheet gaps. The latter were found to dominate the gas transport and yielded a molecular cutoff of 3.6 Å with a H2/N2 selectivity above 20. The gaps were successfully removed by the condensation of the terminal silanol groups of RUB-15 to yield H2/CO2 selectivities up to 100. The high selectivity was exclusively from the transport across 6-MR, which was confirmed by a good agreement between the experimentally determined apparent activation energy of H2 and that computed by ab initio calculations. The scalable fabrication and the attractive sieving performance at 250–300 °C make these membranes promising for precombustion carbon capture.
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U2 - 10.1038/s41563-020-00822-2
DO - 10.1038/s41563-020-00822-2
M3 - Article
C2 - 33020610
AN - SCOPUS:85092088922
SN - 1476-1122
VL - 20
SP - 362
EP - 369
JO - Nature Materials
JF - Nature Materials
IS - 3
ER -