Multi-Template-Guided Synthesis of High-Dimensional Molecular Assemblies for Humidity Gradient-Based Power...

Area of Science:

• Materials Science
• Inorganic Chemistry
• Supramolecular Chemistry

Background:

• Integrating multiple functionalities into molecular assemblies is crucial but challenging due to the dynamic nature of inorganic building blocks.
• Crystal engineering requires precise control over the assembly of these dynamic components.

Purpose of the Study:

• To develop a novel strategy for controlling the assembly of inorganic building blocks into complex molecular structures.
• To explore the potential of these engineered assemblies in energy applications, specifically proton conduction and power generation.

Main Methods:

• A multi-template-guided strategy was employed, utilizing coordination modes of ligands and spatial hindrance of anionic templates.
• Flexible multi-dentate linkers were used to selectively form oligomeric assemblies and tetrahedral cages.
• Anionic templates assisted in assembling cages into Möbius nanobelts.

Main Results:

• The strategy successfully controlled the formation of various molecular assemblies, including tetrahedral cages ({Te4Mo24}, {As4Mo24}) and a Möbius nanobelt ({P8Mo48}).
• The hydrophilic-hydrophobic hybrid cage {Te4Mo24} demonstrated excellent proton conduction properties.
• A humidity gradient-based power generator (HGPG) based on {Te4Mo24}-Poly(vinylidene fluoride) achieved a notable open-circuit voltage (0.51 V) and current density (77.8 nA cm-2) at 90% RH.

Conclusions:

• The multi-template strategy offers a universal approach for synthesizing multifunctional molecular integration molecules.
• {Te4Mo24} serves as a promising prototype for developing efficient humidity gradient-based power generators.
• Molecular dynamics simulations provided insights into water molecule interactions within the generator, aiding further optimization.