Photovoltaic Energy Conversion and Storage of Micro-Supercapacitors Based on Emulsion Self-Assembly of Upconverting Nanoparticles

[Image: see text] With the rapid need for new kinds of portable and wearable electronics, we must look to develop flexible, small-volume, and high-performance supercapacitors that can be easily produced and stored in a sustainable way. An integrated system simultaneously converting recyclable energy to electricity and storing energy is sought after. Here we report photovoltaic energy conversion and storage integrated micro-supercapacitors (MSCs) with asymmetric, flexible, and all-solid-state performances constructed from thousands of close-packed upconverting nanoparticles (UCNPs) via an emulsion-based self-assembly process using oleic acid (OA)-capped upconverting nanoparticles. The carbonated-UCNPs supraparticles (CSPs) are further coated with polypyrrole (PPy) to improve their electrochemical performance. Such a design can develop CSPs@PPy as electrode materials with high gravimetric capacitance, 308.6 F g(–1) at 0.6 A g(–1). The fabricated MSCs exhibit excellent areal capacitance, C(s) = 21.8 mF cm(–2) at 0.36 A cm(–2) and E = 0.00684 mWh cm(–2), and have superior flexibility and cycling ability. The MSC devices have a sensitive near-infrared ray (NIR) photoelectrical response capability, which can capture the NIR of sunlight to convert it into electrical energy and store the electric energy due to an excellent capacitive performance. We propose a method for multifunctional integration of energy conversion and storage, and provide future research directions and potential applications of self-powered flexible wearable photonic electronics.