Intermingled Coordination Environments Enable Defect-Engineered Metal-Polyphenol/G-Quadruplex Hydrogel for Enhanced...

Area of Science:

• Supramolecular Chemistry
• Materials Science
• Catalysis

Background:

• Defect engineering in catalysts is crucial for tuning electronic structure and reactivity.
• Supramolecular assemblies offer unique platforms for creating controlled catalytic environments.

Purpose of the Study:

• To develop a supramolecular strategy for defect engineering in a hydrogel matrix.
• To enhance photocatalytic nitrogen fixation using engineered defects and biomimetic confinement.

Main Methods:

• Confining a Bi3+-caffeic acid complex within a guanosine monophosphate-based G-quadruplex hydrogel.
• Utilizing the G-quadruplex scaffold for ion-channel pathways and uniform catalytic site dispersion.
• Investigating the formation of oxygen-vacancy-rich heterojunctions.

Main Results:

• The engineered hydrogel exhibited an exceptional N2 to NH3 conversion rate of 905.2 µmol h−1 g−1(cat).
• This rate is 3.8 times higher than that of the pristine complex.
• The G-quadruplex hydrogel facilitated charge transport, substrate diffusion, and selective adsorption.

Conclusions:

• The supramolecular approach successfully integrated defect engineering, heterojunction formation, and biomimetic confinement.
• G-quadruplex hydrogels represent a powerful platform for sustainable photocatalytic nitrogen fixation.
• This strategy holds potential for broader applications in catalysis and beyond.