Palladium-Percolated Networks Enabled by Low Loadings of Branched Nanorods for Enhanced H2 Separations

Hu, Leiqing; Chen, Kaiwen; Lee, Won‐Il; Kisslinger, Kim; Rumsey, Clayton; Fan, Shouhong; Bui, Vinh T.; Esmaeili, Narjes; Tran, Thien; Ding, Yifu; Trebbin, Martin; Nam, Chang‐Yong; Swihart, Mark T.; Lin, Haiqing

doi:10.1002/adma.202301007

Palladium-Percolated Networks Enabled by Low Loadings of Branched Nanorods for Enhanced H₂ Separations

Journal Article · Sat Apr 01 00:00:00 EDT 2023 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202301007· OSTI ID:2007528

Hu, Leiqing ^[1]; Chen, Kaiwen ^[1]; ^[2]; Kisslinger, Kim ^[3]; Rumsey, Clayton ^[1]; Fan, Shouhong ^[4]; Bui, Vinh T. ^[1]; Esmaeili, Narjes ^[1]; Tran, Thien ^[1]; Ding, Yifu ^[4]; Trebbin, Martin ^[1]; Nam, Chang‐Yong ^[5]; Swihart, Mark T. ^[1]; ^[1]

State University of New York (SUNY), Buffalo, NY (United States)
Stony Brook University, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
University of Colorado, Boulder, CO (United States)
Stony Brook University, NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Nanoparticles (NPs) at high loadings are often used in mixed matrix membranes (MMMs) to improve gas separation properties, but they can lead to defects and poor processability that impede membrane fabrication. Herein, it is demonstrated that branched nanorods (NRs) with controlled aspect ratios can significantly reduce the required loading to achieve superior gas separation properties while maintaining excellent processability, as demonstrated by the dispersion of palladium (Pd) NRs in polybenzimidazole for H₂/CO₂ separation. Increasing the aspect ratio from 1 for NPs to 40 for NRs decreases the percolation threshold volume fraction by a factor of 30, from 0.35 to 0.011. An MMM with percolated networks formed by Pd NRs at a volume fraction of 0.039 exhibits H₂ permeability of 110 Barrer and H₂/CO₂ selectivity of 31 when challenged with simulated syngas at 200 °C, surpassing Robeson's upper bound. In conclusion, this work highlights the advantage of NRs over NPs and nanowires and shows that right-sizing nanofillers in MMMs is critical to construct highly sieving pathways at minimal loadings. In conclusion, this work paves the way for this general feature to be applied across materials systems for a variety of chemical separations.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: FE0031636; FE0032209; SC0012704

OSTI ID:: 2007528

Alternate ID(s):: OSTI ID: 1983471

Report Number(s):: BNL--224867-2023-JAAM

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 26 Vol. 35; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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