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PreprintCC BYChemRxiv

Shaping single crystals through a controlled non-classical crystallization pathway

  • Thao Nguyen1,2,3
  • João Pedro Vale4,5
  • Oriol Arteaga6
  • Annalisa Calò7,2,8
  • James D. Nicholas1,2,3
  • Roc Matheu1,2,9
  • Mario Palacios-Corella1,2,3
  • Andriu Cavegn3,2
  • Maria Guix1,2,3
  • Alessandro Sorrenti1,2,10
  • Salvador Pané11,12
  • Tiago Sotto Mayor4,5
1 more authors
  • Josep Puigmartí-Luis1,2,3,13
13 affiliations
  1. 1Institut de Química Teòrica i Computacional
  2. 2University of Barcelona (UB)
  3. 3Departament de Ciència dels Materials i Química Física
  4. 4Faculty of Engineering
  5. 5CEFT - Transport Phenomena Research Center, ALiCE - Associate Laboratory in Chemical Engineering, University of Porto
  6. 6Departament de Fisica Aplicada, Universitat de Barcelona, IN2UB, Barcelona, Spain, 08028
  7. 7Department of Electronic and Biomedical Engineering
  8. 8Institute for Bioengineering of Catalonia (IBEC)
  9. 9Departament de Química Inorgànica i Orgànica, (Secció de Química Inorgànica
  10. 10Departament de Química Inorgànica i Orgànica, (Secció de Química Orgànica
  11. 11Institute of Robotics and Intelligent Systems
  12. 12Multi-Scale Robotics Lab, ETH Zürich
  13. 13Institució Catalana de Recerca i Estudis Avançats (ICREA)
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Abstract

The ability to program the shape of single crystals through molten-state processing has transformed the manufacturing of inorganic materials, yet this strategy is fundamentally incompatible with most organic-based crystals, which decompose before melting. Here, we show that a non-classical crystallization pathway can overcome this limitation by generating a moldable dense-liquid intermediate during the growth of peptide-based metal-organic frameworks (MOFs). By engineering a reaction environment in which precursor concentration and reagent diffusion are controlled while suppressing convection, we selectively activate a liquid-liquid phase separation process to produce a confined dense-liquid phase that can be shaped prior to crystallization. Repeated diffusion-limited chemical perturbations subsequently transform this intermediate into single crystals that faithfully preserve the geometry of the confined environment in which they form, enabling non-equilibrium morphologies inaccessible by conventional synthesis. We further show that crystal shape influences mechanical properties, demonstrating that controlling crystallization pathways provides a route to tailor function without altering chemical composition.

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Cite

BibTeXRIS
BibTeX
@misc{nguyen2026shaping,
  title = {{Shaping single crystals through a controlled non-classical crystallization pathway}},
  author = {Thao Nguyen and João Pedro Vale and Oriol Arteaga and Annalisa Calò and James D. Nicholas and Roc Matheu and Mario Palacios-Corella and Andriu Cavegn and Maria Guix and Alessandro Sorrenti and Salvador Pané and Tiago Sotto Mayor and Josep Puigmartí-Luis},
  howpublished = {ChemRxiv},
  year = {2026},
  month = oct,
  doi = {10.26434/chemrxiv.15009961/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009961/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Shaping single crystals through a controlled non-classical crystallization pathway
AU  - Thao Nguyen
AU  - João Pedro Vale
AU  - Oriol Arteaga
AU  - Annalisa Calò
AU  - James D. Nicholas
AU  - Roc Matheu
AU  - Mario Palacios-Corella
AU  - Andriu Cavegn
AU  - Maria Guix
AU  - Alessandro Sorrenti
AU  - Salvador Pané
AU  - Tiago Sotto Mayor
AU  - Josep Puigmartí-Luis
PY  - 2026
DA  - 2026/10/06
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15009961/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009961/v1
AB  - The ability to program the shape of single crystals through molten-state processing has transformed the manufacturing of inorganic materials, yet this strategy is fundamentally incompatible with most organic-based crystals, which decompose before melting. Here, we show that a non-classical crystallization pathway can overcome this limitation by generating a moldable dense-liquid intermediate during the growth of peptide-based metal-organic frameworks (MOFs). By engineering a reaction environment in which precursor concentration and reagent diffusion are controlled while suppressing convection, we selectively activate a liquid-liquid phase separation process to produce a confined dense-liquid phase that can be shaped prior to crystallization. Repeated diffusion-limited chemical perturbations subsequently transform this intermediate into single crystals that faithfully preserve the geometry of the confined environment in which they form, enabling non-equilibrium morphologies inaccessible by conventional synthesis. We further show that crystal shape influences mechanical properties, demonstrating that controlling crystallization pathways provides a route to tailor function without altering chemical composition.
ER  -