Closed‐Loop Recyclable Polyhexahydrotriazine Aerogels Utilizing N,N‐Dimethyl Lactamide as a Green Solvent

Chang‐lin Wang; Ivona Glišić; Yi‐Ru Chen; Željko Tomović

doi:10.1002/cssc.202500125

journal article Open Access Jun 03, 2025

Closed‐Loop Recyclable Polyhexahydrotriazine Aerogels Utilizing N,N‐Dimethyl Lactamide as a Green Solvent

Chang‐lin Wang

Ivona Glišić

Yi‐Ru Chen

Željko Tomović

ChemSusChem Vol. 18 No. 14 · Wiley

View at Publisher Save 10.1002/cssc.202500125

Abstract

Organic aerogels, known for their lightweight, highly porous structure, and ultralow thermal conductivity, have shown great potential in thermal insulation, chemical absorption, and energy storage. However, most aerogels to date pose environmental concerns, as their permanently cross‐linked scaffold makes recycling back to the original monomers virtually impossible. Additionally, the use of toxic solvents in aerogel fabrication raises further environmental and health concerns, challenging their sustainable application. Moreover, the development of next‐generation organic aerogels requires the design of recyclable materials with improved mechanical properties. In response to these challenges, this study demonstrates the synthesis of chemically recyclable polyhexahydrotriazine (PHT) aerogels based on an amide containing aromatic diamine, utilizing N,N‐dimethyl lactamide, a nontoxic and label‐free solvent, as gelation medium. Hansen solubility parameters provide key insights into how solvent choice influences the morphology and properties of PHT aerogels. The resulting PHT aerogels exhibit low bulk density (≈63 mg cm−3), high porosity (≈96%), excellent thermal insulation properties (≈17 mWm−1 K−1), and enhanced mechanical performance, all while being closed‐loop recyclable. This work highlights the importance of solvent selection in tuning aerogel properties and demonstrates a green route for fabricating sustainable, high‐performance thermal insulating materials.

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Details

Published: Jun 03, 2025
Vol/Issue: 18(14)
License: View

Authors

C

Chang‐lin Wang

Department Polymer Performance Materials Group Department of Chemical Engineering and Chemistry Institute for Complex Molecular Systems (ICMS) Eindhoven University of Technology 5600 MB Eindhoven The Netherlands

I

Ivona Glišić

Department Polymer Performance Materials Group Department of Chemical Engineering and Chemistry Institute for Complex Molecular Systems (ICMS) Eindhoven University of Technology 5600 MB Eindhoven The Netherlands

Y

Yi‐Ru Chen

Department Polymer Performance Materials Group Department of Chemical Engineering and Chemistry Institute for Complex Molecular Systems (ICMS) Eindhoven University of Technology 5600 MB Eindhoven The Netherlands

�

Željko Tomović

Department Polymer Performance Materials Group Department of Chemical Engineering and Chemistry Institute for Complex Molecular Systems (ICMS) Eindhoven University of Technology 5600 MB Eindhoven The Netherlands

Funding

European Cooperation in Science and Technology Award: ECO‐AEROGELS IG18125

Cite This Article

Chang‐lin Wang, Ivona Glišić, Yi‐Ru Chen, et al. (2025). Closed‐Loop Recyclable Polyhexahydrotriazine Aerogels Utilizing N,N‐Dimethyl Lactamide as a Green Solvent. ChemSusChem, 18(14). https://doi.org/10.1002/cssc.202500125

Closed‐Loop Recyclable Polyhexahydrotriazine Aerogels Utilizing N,N‐Dimethyl Lactamide as a Green Solvent

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