Channel Microenvironment‐Controlled Pillared <scp>MOF</scp> as Efficient Triboelectric Nanogenerator Material for Self‐Powered Degradation of Organic Pollutants

The development of metal–organic framework triboelectric materials is crucial for applying nanomaterials to new energy conversion technologies. This work utilized the SC‐SC ligand substitution method to regulate the 3D MOF pore channel environment, thereby generating a hierarchical framework structure composed of bridging ligands with different conjugation levels. The triboelectric generation experimental results showed that ZUT‐10‐bpe has excellent output capabilities with a short‐circuit current of 116.14 μA and a power density of 4531.52 mW m −2 , respectively. The density functional theory results indicated that ZUT‐10‐bpe has the smallest HOMO‐LUMO band gap and the highest HOMO energy level. The combined density of states calculation and multiphysics field simulation confirmed that introducing organic ligands with π conjugation systems and adjusting the degree of planar conjugation can significantly enhance electron generation and improve electron transfer, thereby significantly improving the triboelectric activity. Additionally, the self‐powered pollution degradation experiment demonstrated that ZUT‐10‐bpe@TENG has a degradation efficiency of over 96% for various organic dyes within 90 min. This research provides a new perspective for MOF‐based TENG in water pollution treatment.