Multilayer Polypyrrole Nanosheets with Self‐Organized Surface Structures for Flexible and Efficient Solar–Thermal Energy Conversion

Converting solar energy into concentrated heat is very appealing for various applications. Polypyrrole (PPy) is known to possess excellent photothermal property with low thermal conductivity, and thus is an ideal candidate for solar-thermal energy conversion. However, solar-thermal materials based on PPy or other conducting polymers still exhibit limited energy conversion efficiency due to the lack of effective light-trapping schemes. Here, it is demonstrated that multilayer PPy nanosheets with spontaneously formed surface structures such as wrinkles and ridges via sequential polymerization on paper substrates can dramatically enhance broadband and wide-angle light absorption across the full solar spectrum, leading to an impressive solar-thermal conversion efficiency of 95.33%. The intriguing solar-thermal properties and structural features of multilayer PPy nanosheets can be used for solar heating and photoactuators. Meanwhile, when used for solar steam generation, the measured efficiency could achieve ≈92% under one sun irradiation. The hierarchically multilayer structure is mechanically flexible and robust, holding great potential for practical solar energy utilization. This study provides a simple and straightforward approach toward engineering light-weight and thermally insulating polymers into efficient solar-thermal materials for emerging solar energy-related applications.