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Alfonso Bayón-Fernández1, Alba Torrón-Celada1, Alejandro Méndez-Ardoy2

  • 1Centro Singular de Investigación en Química Biolóxica e Materiais Moleculares (CIQUS) and Departamento de Química Orgánica, Universidade de Santiago de Compostela, Rúa de Jenaro de la Fuente, s/n, 15705, Santiago de Compostela, Spain.

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Researchers created novel light-emitting two-dimensional (2D) nanosheets using pH-responsive cyclic peptide-tetraphenylethene (TPE) building blocks. This breakthrough enables precise control over 2D material assembly and function, opening doors for new supramolecular materials.

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2D MaterialsAggregation‐induced EmissionCatalysisCyclic PeptidesSelf‐assembly

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Area of Science:

  • Supramolecular Chemistry
  • Materials Science
  • Nanotechnology

Background:

  • Two-dimensional (2D) materials and aggregation-induced emission (AIE) fluorophores offer unique properties.
  • Integrating AIE probes into 2D self-assembled systems with nanometric control is challenging due to assembly sensitivity.

Purpose of the Study:

  • To develop a novel scaffold for creating light-emitting 2D materials by combining AIE fluorophores with self-assembling cyclic peptides (CPs).
  • To achieve nanometric control over the self-assembly of AIE-functionalized 2D materials.

Main Methods:

  • Synthesized tetrakis-(cyclopeptide) tetraphenylethene monomers using oxime bond connections.
  • Exploited pH-dependent self-assembly of these monomers to form 2D macrotubular nanoarrays.
  • Investigated the impact of molecular modifications on the TPE core and CP units on self-assembly and material properties.

Main Results:

  • Achieved pH-dependent self-assembly of TPE-CP monomers into light-emitting 2D nanosheets.
  • Demonstrated that the tetrameric CP motif tolerates diverse molecular modifications without disrupting 2D self-assembly.
  • Showcased precise height control of the 2D nanosheets by adjusting the TPE core structure.
  • Utilized the aligned histidine residues for enzyme mimicry, demonstrating esterase activity.

Conclusions:

  • The developed TPE-CP scaffold enables the creation of functional 2D supramolecular materials with tunable properties.
  • The system's tolerance to molecular diversity facilitates the design of new advanced materials.
  • This work provides a versatile platform for constructing sophisticated 2D nanoarchitectures with potential applications in catalysis and sensing.