Integrating Dual-Interfacial Liquid Metal Based Nanodroplet Architectures and Micro-Nanostructured Engineering for High Efficiency Solar Energy Harvesting

Broadband strong absorption of solar light over a wide range of angles, low heat loss, and excellent structural reliability are of significance for enhancing solar harvesting of photothermal materials; however, it remains a challenge to achieve these attributes simultaneously. Herein, a tailored photothermal composite nanodroplet (LMP-rGO) featured with dual-interface, which comprises liquid metal (LM) core with polydopamine (PDA) photothermal middle layer of tunable thickness and reduced graphene oxide (rGO) shell, is particularly prepared. Thermal-insulating PDA coating and light-absorbing carbonaceous shell allow it to synergistically suppress heat loss and reinforce photon absorptivity. To maximize photothermal conversion and photon harvesting yield on solar light, inspired by light trapping architecture, a three-dimensional (3D) stepped micropyramid grating array framework is tactfully designed to ameliorate light coupling. Utilizing the scalability and cost-effectiveness of the poly(vinyl alcohol) (PVA), the flexible 3D-structured PVA/LMP-rGO absorbers are successfully constructed via a controllable casting molding strategy. As a proof-of-concept, the developed micrograting absorber exhibits a desirable combination of strong broadband selective light absorption (94.9% for parallel to the grating direction and 97.3% for perpendicular to the grating direction), superior photothermal conversion effect (89.4%), high heat flux density, and fascinating mechanical properties. Also, an efficient and steady solar-driven thermoelectric generator (STEG) system for real-time solar-heat-electric conversion, with its high peak power density of 245.9 μW cm^-2 under one sun irradiation, is further displayed, making an important step to rationally design LM-based nanocomposite droplets for solar energy harvesting.