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Making and Breaking Supramolecular Synthons for Modular Protein Frameworks.

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Summary
This summary is machine-generated.

Anionic calixarenes mediate protein assembly. Replacing sulfonato-calix[8]arene with phosphonato-calix[6]arene in Ralstonia solanacearum lectin assemblies controls crystal formation, demonstrating synthon durability

Keywords:
affinity tagcrystal engineeringmacrocyclerecognitionself‐assembly

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Area of Science:

  • Supramolecular chemistry
  • Protein crystallography
  • Materials science

Background:

  • Anionic calixarenes are key in directing protein self-assembly into crystalline structures.
  • Ralstonia solanacearum lectin (RSL) exhibits pH-dependent cocrystallization with p-sulfonato-calix[8]arene (sclx8), forming multiple polymorphs.
  • The sclx8 dimer acts as a supramolecular synthon, influencing the resulting crystal architecture.

Purpose of the Study:

  • To investigate the effect of replacing sclx8 with p-phosphonato-calix[6]arene (pclx6) on RSL assembly.
  • To determine if pclx6 can yield a single, stable cocrystal form.
  • To explore the role of calixarene type and synthon durability in protein crystal engineering.

Main Methods:

  • Cocrystallization experiments using RSL and pclx6 under various pH and crystallization conditions.
  • Structural analysis of the resulting RSL-pclx6 cocrystals.
  • Comparative studies with RSL-sclx8 cocrystals.
  • Investigation using a mutant RSL with an affinity tag for macrocycle binding.
  • Ternary mixture experiments with RSL, pclx6, and sclx8.

Main Results:

  • RSL-pclx6 cocrystallization consistently yielded a single crystal form, irrespective of pH or conditions, contrasting with sclx8.
  • The pclx6 dimer proved more durable, dictating assembly and polymorph selection.
  • A mutant RSL with an affinity tag formed an altered, porous framework with pclx6.
  • Ternary mixtures demonstrated pH-driven self-sorting between RSL, pclx6, and sclx8.

Conclusions:

  • The type of calixarene (phosphonate vs. sulfonate) significantly influences supramolecular synthon durability and protein assembly outcomes.
  • Calixarene synthon choice offers a powerful strategy for controlling protein crystal engineering and polymorph selection.
  • The "mix-and-match" approach using proteins and supramolecular synthons is a promising avenue for designing novel protein-based materials.