Construction of supramolecular metal-halogen bonded organic frameworks for efficient solar energy conversion

Efficient conversion and synergistic solar energy utilization are critical for advancing low-carbon and sustainable development. In this study, two Pt(II)-based metal/halogen-bonded organic frameworks (MXOF-Ben and MXOF-Anth) were designed to enhance photoconversion efficiency and enable multifunctional integration. The ligand L-terpyr is formed by coupling tripyridine with diphenylamine dipyridine, in which the tripyridine effectively acts as a metal-ligand to lower the band gap and promote non-radiative leaps, thereby enhancing the photoconversion ability. Meanwhile, diphenylamine dipyridine serves as a [N⋯I⁺⋯N] halogen-bonding acceptor, imparting superhydrophilicity to the materials and increasing carrier density, further improving photocatalytic performance. Experimental results demonstrate that these two MXOFs achieve impressive interfacial water evaporation efficiencies of up to 87.8% and 94.0%, respectively. Additionally, the materials exhibit excellent performance in photothermal power generation and photocatalysis of H₂O₂. Notably, the MXOFs also deliver strong overall performance in integrated systems combining interfacial water evaporation with photothermal power generation or photocatalysis, underscoring their exceptional photoconversion efficiency and multifunctional potential. This work introduces a novel strategy by incorporating metal-ligand and halogen bonds, offering a pathway to enhance photoconversion efficiency and develop versatile materials for advanced solar energy applications, thereby fostering the progress of high-efficiency solar energy conversion and multifunctional organic materials.