Organic Dye-Modified Two-Dimensional Metal–Organic Framework/Carbon Nanotube Composite Films for Photothermoelectric Applications

High Resolution Image Download MS PowerPoint Slide Photothermoelectric (PTE) systems, which convert light into electricity through sequential photothermal (PT) and thermoelectric (TE) processes, offer a promising strategy for self-powered wearable electronics. In this work, we develop a homogeneous PTE composite system by integrating carbon nanotubes (CNTs) with a dye-modified two-dimensional metal–organic framework (2D MOF), referred to as ZrBTBD, obtained via the postsynthetic modification of a 2D MOF, ZrBTB, with N719 dye. The introduction of N719 enhances visible-light absorption and facilitates doping level modulation with CNTs. Together with n-type doping using N-DMBI, the resulting p-type C/ZrBTBD10 and n-type C/ZrBTBD-N5 composites achieve high power factors of 465.7 and 363.1 μW m –1 K –2, respectively. Under 100 mW cm –2 illumination, the PT temperature increases from 47.3 °C to 51.2 °C, and the zT is significantly enhanced compared to CNTs. A flexible PTE generator assembled from these composites delivers an open-circuit voltage of 12.3 mV and a maximum power output of 365.4 nW. A wearable prototype demonstrates its potential for flexible, self-powered electronics. This work represents the demonstration of dye-immobilized MOF/CNT composite materials in PTE systems, offering a molecular-level strategy for integrating light harvesting, interfacial charge modulation, and thermoelectric conversion.