Janus Photothermal Films with Orientated Plasmonic Particle-in-Cavity Surfaces Enabling Heat Control in Solar-Thermal-Electric Generators

Solar thermoelectric generators (STEGs) consisting of solar absorbers and thermoelectric generators (TEGs) can utilize solar energy to generate electrical power. However, performances of STEGs are limited by the heat losses of solar absorbers in air, which become more and more significant with an increase in the solar absorbing area. Herein, we describe the preparation of Au@AgPd nanostructure monolayer/poly(vinyl alcohol) (PVA) Janus photothermal films with broadband plasmonic absorption in the visible and near-infrared regions. By uniaxially stretching the Janus film, Au@AgPd can align along the stretching direction, which creates particle-in-cavity structures on the PVA surface. Benefiting from the oriented plasmonic particle-in-cavity configuration, the Janus films effectively convert sunlight into heat, trap the heat within their micrometer-depth structure, and facilitate its transfer along the direction of the nanostructure orientation. Integration of the Janus films with commercial TEGs allows thermal concentration onto a small thermoelectric surface, yielding an open-circuit voltage of 308 mV under 102 mW/cm² natural sunlight illumination. Heat losses in commercial TEGs integrated with Janus films are reduced by approximately 50% while maintaining the same voltage output. Furthermore, incorporating the Janus films into a conventional STEG with carbon-based solar absorbers significantly enhances solar-thermal-electric conversion performance, achieving an output power density of 1.3 W m^–2. Our design of Janus photothermal films with oriented particle-in-cavity surfaces can be extended to various solar-thermal systems for high-efficiency solar energy conversion and heat management.