Atomically Fine-Tuning Organic–Inorganic Carbon Molecular Sieve Membranes for Hydrogen ProductionClick to copy article linkArticle link copied!
- Leiqing HuLeiqing HuDepartment of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York 14260, United StatesMore by Leiqing Hu
- Won-Il LeeWon-Il LeeDepartment of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11794, United StatesMore by Won-Il Lee
- Kai ChenKai ChenDepartment of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York 14260, United StatesMore by Kai Chen
- Soumyabrata RoySoumyabrata RoyDepartment of Materials Science and NanoEngineering, Rice University, Houston, Texas 77005, United StatesDepartment of Sustainable Energy Engineering, Indian Institute of Technology Kanpur, Kanpur, Uttar Pradesh 208016, IndiaMore by Soumyabrata Roy
- Kieran FungKieran FungDepartment of Mechanical Engineering, University of Colorado, Boulder, Colorado 80309, United StatesMore by Kieran Fung
- Kim KisslingerKim KisslingerCenter for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United StatesMore by Kim Kisslinger
- Erda DengErda DengDepartment of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York 14260, United StatesMore by Erda Deng
- Yifu DingYifu DingDepartment of Mechanical Engineering, University of Colorado, Boulder, Colorado 80309, United StatesMore by Yifu Ding
- Pulickel M. AjayanPulickel M. AjayanDepartment of Materials Science and NanoEngineering, Rice University, Houston, Texas 77005, United StatesMore by Pulickel M. Ajayan
- Chang-Yong Nam*Chang-Yong Nam*Email: [email protected]Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11794, United StatesCenter for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United StatesMore by Chang-Yong Nam
- Haiqing Lin*Haiqing Lin*Email: [email protected]Department of Chemical and Biological Engineering, University at Buffalo, The State University of New York, Buffalo, New York 14260, United StatesMore by Haiqing Lin
Abstract

Polymeric membranes with great processability are attractive for the H2/CO2 separation required for hydrogen production from renewable biomass with carbon capture for utilization and sequestration. However, it remains elusive to engineer polymer architectures to obtain desired sub-3.3 Å ultramicropores to efficiently sieve H2 from CO2. Herein, we demonstrate a scalable way of carbonizing polybenzimidazole (PBI) at low temperatures, followed by vapor phase infiltration (VPI) to atomically narrow ultramicropores throughout the films, forming hybrid organic–inorganic carbon molecular sieves (CMSs). One VPI cycle (100 s) for the PBI carbonized at 500 °C remarkably increases H2/CO2 selectivity from 9.6 to 83 at 100 °C, surpassing Robeson’s upper bound. The CMS demonstrates a stable H2/CO2 separation performance when challenged with simulated syngas streams and can be fabricated into thin-film composite membranes, outperforming state-of-the-art membranes. The scalable approach can be ubiquitous to molecularly fine-tune ultramicropores of leading polymeric membranes to further improve their size-sieving ability and thus separation efficiency.
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