<p>Solvent reverse osmosis is a pressure-driven, liquid-phase process for separating solvent mixtures, offering a potential low-energy alternative to thermal operations. Graphene oxide (GO) laminates provide tunable nanochannels to probe confined solvent transport, yet solvent–solvent separations remain underexplored due to solvation-induced structural instabilities and the small molecular sizes. Here we construct solvent-stable, supported GO nanochannel membranes that preserves integrity under pressurized solvents, and tune interlayer confinement and surface polarity via controlled chemical reduction. Across 51 solvent systems and 5 distinct nanochannels, we demonstrate that separation is governed by coupled nanoconfinement and solvent affinity, where selective interfacial association can surpass simple size-exclusion expectations. Maximum permselectivity arises from balancing channel size with retained polarity, indicating that channel shrinking alone does not optimize performance. These findings identify channel surface chemistry as a key design factor for polarity-rich solvent systems and provide a framework for rationally tailoring nanochannels for complex solvent separations.</p>

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Solvent reverse osmosis beyond size exclusion in two-dimensional nanochannel membranes

  • Kecheng Guan,
  • Yuanyuan Guo,
  • Liheng Dai,
  • Aiwen Zhang,
  • Zhan Li,
  • Erda Deng,
  • Keizo Nakagawa,
  • Yanan Guo,
  • Gongping Liu,
  • Tomohisa Yoshioka,
  • Wanqin Jin,
  • Hideto Matsuyama

摘要

Solvent reverse osmosis is a pressure-driven, liquid-phase process for separating solvent mixtures, offering a potential low-energy alternative to thermal operations. Graphene oxide (GO) laminates provide tunable nanochannels to probe confined solvent transport, yet solvent–solvent separations remain underexplored due to solvation-induced structural instabilities and the small molecular sizes. Here we construct solvent-stable, supported GO nanochannel membranes that preserves integrity under pressurized solvents, and tune interlayer confinement and surface polarity via controlled chemical reduction. Across 51 solvent systems and 5 distinct nanochannels, we demonstrate that separation is governed by coupled nanoconfinement and solvent affinity, where selective interfacial association can surpass simple size-exclusion expectations. Maximum permselectivity arises from balancing channel size with retained polarity, indicating that channel shrinking alone does not optimize performance. These findings identify channel surface chemistry as a key design factor for polarity-rich solvent systems and provide a framework for rationally tailoring nanochannels for complex solvent separations.