<p>Two-dimensional framework membranes (2DFMs) hold great promise for sustainable energy-harvesting technologies, yet their performance is often limited by low electric double-layer (EDL) coverage (<i>ƞ</i><sub><i>EDL</i></sub>) arising from large channels and/or low charge densities. Here, we report an ultrathin ( ~ 50 nm), fully crystalline, ABC-stacked viologen-incorporated 2D polymer membrane (sV2DP) featuring vertically aligned triangular nanochannels (<i>D</i><sub><i>eff</i></sub> = 1.36 nm) densely decorated with pyridinium sites ( + 22.4 mC m<sup>−2</sup>). Compared with its non-staggered AA-stacked analogue, sV2DP exhibits a 3.2-fold enhancement in <i>ƞ</i><sub><i>EDL</i></sub> under a 50-fold KCl gradient, combining high anionic selectivity (<i>t</i><sub>− </sub>= 0.85) with remarkable selective current density (14.6 kA m<sup>−2</sup>). Simulations reveal that spirally arranged charges generate a unique “screw-like” anion migration pathway, significantly enhancing transmembrane efficiency relative to non-staggered 2DP analogues. When integrated into micro-aperture osmotic power generators, the sV2DP membrane delivered a peak power density of 243 W m<sup>−2</sup> under a 50-fold NaCl gradient, placing it among the highest-performing systems.</p>

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Ultranarrow nanochannels in a staggered two-dimensional polymer membrane enhance electric double-layer coverage for osmotic energy harvesting

  • Feng Ni,
  • Ye Yang,
  • Shuangjie Zhao,
  • Mahabir Prasad,
  • Naveen Goyal,
  • Xusheng Yang,
  • Dongxu Wang,
  • Jianjun Zhang,
  • Mike Hambsch,
  • Miroslav Polozij,
  • Stefan C. B. Mannsfeld,
  • Ute Kaiser,
  • Grégory F. Schneider,
  • Thomas D. Kühne,
  • Thomas Heine,
  • Zhiyong Wang,
  • Xinliang Feng

摘要

Two-dimensional framework membranes (2DFMs) hold great promise for sustainable energy-harvesting technologies, yet their performance is often limited by low electric double-layer (EDL) coverage (ƞEDL) arising from large channels and/or low charge densities. Here, we report an ultrathin ( ~ 50 nm), fully crystalline, ABC-stacked viologen-incorporated 2D polymer membrane (sV2DP) featuring vertically aligned triangular nanochannels (Deff = 1.36 nm) densely decorated with pyridinium sites ( + 22.4 mC m−2). Compared with its non-staggered AA-stacked analogue, sV2DP exhibits a 3.2-fold enhancement in ƞEDL under a 50-fold KCl gradient, combining high anionic selectivity (t− = 0.85) with remarkable selective current density (14.6 kA m−2). Simulations reveal that spirally arranged charges generate a unique “screw-like” anion migration pathway, significantly enhancing transmembrane efficiency relative to non-staggered 2DP analogues. When integrated into micro-aperture osmotic power generators, the sV2DP membrane delivered a peak power density of 243 W m−2 under a 50-fold NaCl gradient, placing it among the highest-performing systems.