Manipulation of the Self-Assembly Morphology by Side-Chain Engineering of Quinoxaline-Substituted Organic Photothermal Molecules for Highly Efficient Solar-Thermal Conversion and Applications

Organic photothermal materials have attracted increasing attention because of their structural diversity, flexibility, and compatibility. However, their energy conversion efficiency is limited owing to the narrow absorption spectrum, strong reflection/transmittance, and insufficient nonradiative decay. In this study, two quinoxaline-based D-A-D-A-D-type molecules with ethyl (BQE) or carboxylate (BQC) substituents were synthesized. Strong intramolecular charge transfer provided both molecules with a broad absorption range of 350-1000 nm. In addition, the high reorganization energy and weak molecular packing of BQE resulted in efficient nonradiative decay. More importantly, the self-assembly of BQE leads to a textured surface and enhances the light-trapping efficiency with significantly reduced light reflection/transmittance. Consequently, BQE achieved an impressive solar-thermal conversion efficiency of 18.16 % under 1.0 kW m-2 irradiation with good photobleaching resistance. Based on this knowledge, the water evaporation rate of 1.2 kg m-2 h-1 was attained for the BQE-based interfacial evaporation device with an efficiency of 83 % under 1.0 kW m-2 simulated sunlight. Finally, the synergetic integration of solar-steam and thermoelectric co-generation devices based on BQE was realized without significantly sacrificing solar-steam efficiency. This underscores the practical applications of BQE-based technology in effectively harnessing photothermal energy. This study provides new insights into the molecular design for enhancing light-trapping management by molecular self-assembly, paving the way for photothermal-driven applications of organic photothermal materials. Two organic molecules BQC and BQE with different substituents on the quinoxaline unit have been designed, with BQE having an ethyl group exhibiting efficient nonradiative decay. Moreover, the self-assembly property of BQE results in a textured surface and thus an efficient light-trapping system. A water-electricity cogeneration device based on BQE was fabricated and showed a water evaporation efficiency of 68 %. image