Charge-Directed Nanocellulose Assembly for Interfacial Phase-Transfer Catalysis.
basic_science · Level V
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- Record sourced from PubMed, PMID 40099434.
- Also identified by DOI 10.1002/adma.202418325.
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Abstract
Liquid-liquid interfaces present unique opportunities for sustainable biphasic catalysis, yet concurrent amplification of molecular transport and reactivity at these boundaries remains challenging. Here it is demonstrated that high-aspect-ratio cationic nanocellulose (HNC<sup>+</sup>) spontaneously self-assembles into mechanically robust nanomesh architectures at oil-water interfaces through charge-directed assembly. This assembly is driven by electrostatic attraction between the cationic nanofibers and the intrinsic negative charge at hydrophobic-aqueous interfaces (σ ≈-0.3 C m<sup>-2</sup>), generating sufficient excess attractive force (ΔU ≈-1,200 k<sub>B</sub>T) to overcome image charge repulsion. The resulting nanomesh exhibits uniform "breathing holes" (≈34 nm) and exceptional stability under extreme conditions (pH 2-13, 1.8 m NaCl, and 90 °C). When applied to oxidative desulfurization, the system achieves >90% thiophene removal under ambient conditions with exceptional atom economy (E-factor < 1.1) and catalyst stability through multiple cycles. This breakthrough strategy for interfacial engineering using renewable materials opens new possibilities for green chemical manufacturing while providing fundamental insights into charge-mediated assembly at liquid interfaces. These findings establish a viable pathway for sustainable heterogeneous catalysis that aligns with circular economy principles.