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Molecular-Level Engineering of Interlayer Channels in Vertically-Aligned LDH Arrays for Efficient Hydrogen

Wenji Zheng1, Yuxin Wang1, Kaiyi Lai1

  • 1State Key Laboratory of Fine Chemicals, R&D Center of Membrane Science and Technology, School of Chemical Engineering, Ocean and Life Sciences, Dalian University of Technology, Panjin, Liaoning, P. R. China.

Small (Weinheim an Der Bergstrasse, Germany)
|May 11, 2026
PubMed
Summary

This study introduces advanced 2D layered double hydroxide (LDH) composite membranes for efficient hydrogen (H2) and carbon dioxide (CO2) separation. The novel membrane design significantly enhances H2 permeance and H2/CO2 selectivity, surpassing previous benchmarks.

Keywords:
H2 separation: interlayer engineeringlayered double hydroxidevertical alignment

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Area of Science:

  • Materials Science
  • Chemical Engineering
  • Membrane Technology

Background:

  • Existing 2D layered double hydroxide (LDH) composite membranes face challenges in orientation control and substrate compatibility for gas separation.
  • Limitations include insufficient accuracy in controlling LDH orientation and poor interfacial adhesion with organic substrates, hindering performance.
  • There is a need for improved membrane designs to enhance gas separation efficiency, particularly for hydrogen purification.

Purpose of the Study:

  • To develop a molecular-level channel engineering strategy for constructing advanced LDH composite membranes.
  • To synergistically integrate vertical orientation, interlayer ion intercalation, and surface chemisorption for enhanced gas separation.
  • To improve both hydrogen permeance and hydrogen/carbon dioxide selectivity beyond the Robeson upper bound.

Main Methods:

  • Hydrothermal growth of LDH vertically on a hydrophilic HPAN substrate, controlling crystal plane orientation.
  • Interlayer ion intercalation using chloride ions (Cl-) to precisely adjust interlayer spacing for selective sieving.
  • Covalent grafting of polyethyleneimine (PEI) onto the LDH surface to introduce CO2 chemisorption sites.

Main Results:

  • Vertically grown LDH on HPAN substrate formed straight-through transfer channels with low tortuosity.
  • Cl- intercalation adjusted interlayer spacing to 0.306 nm, facilitating H2/CO2 sieving.
  • LDH(Cl-)/PEI-HPAN membranes achieved 707 GPU H2 permeance and 78.5 H2/CO2 selectivity, exceeding the 2008 Robeson upper bound.

Conclusions:

  • The synergistic integration of vertical orientation, Cl- intercalation, and PEI chemisorption significantly enhances membrane performance.
  • The prepared membranes exhibit excellent H2 permeance and H2/CO2 selectivity due to optimized channel structure and surface chemistry.
  • This approach offers a new paradigm for designing high-performance, scalable 2D material membranes for industrial hydrogen purification.