Thermoelectric power generation from solar radiation or waste heat has attracted tremendous attention due to strong global demand for cost-effective, pollution-free forms of energy conversion. However, the storage and sustainable release of thermal energy, as essential factors for thermoelectric generators (TEGs), remain great challenges. Herein, a TEG based on phase change aerogels (PCAs) has been fabricated to enhance the solar–thermal–electric energy conversion. The PCAs exhibit synergistic phase change properties, excellent thermal reliability, and shape-stabilized properties and can overcome the drawbacks of enthalpy degradation and leakage existing in the phase change materials (PCMs). Under the radiation of simulated solar light, the voltage and current output of the PCA-loaded TEG (∼144 mV, 14.8 mA) are approximately 3 times and 2.7 times that of a blank one (∼48 mV, 5.4 mA), respectively, and the thermal-to-electricity conversion maximum efficiency is enhanced by about 61.3% compared to that of the blank one. The sustained thermal release based on PCAs enables a sustainable electric output when solar light or the heat source is removed. In proof-of-concept experiments, the PCA-loaded TEGs can instantly light up commercial LEDs, drive various portable electronic gadgets, and charge several different capacitors. The sustainable lighting time of eighty green LEDs directly powered by PCA-loaded TEGs is about 4 times longer than that of the blank one. In particular, the maximum value of the voltage difference (ΔV) of LEDs powered by PCA-loaded TEGs and the blank one is up to 1.74 V. Therefore, the PCA-loaded TEGs have enhanced power supply capability when removing solar radiation or the heat source. This study expands the application of PCMs in TEGs and promises a new potential application in advanced energy-related devices and systems for solar energy utilization and storage, self-powered sensing systems, waste heat reuse and other fields.

Triboelectric nanogenerator (TENG) can convert tiny mechanical energy into precious electrical energy. Constant improvements to the output performance of TENG is not only the driving force for its sustainable development, but also the key to expand its practical applicability in modern smart devices. However, most previous studies were conducted at room temperature, ignoring the influence of temperature on the output performance of TENG. Additionally, due to thermionic emission effect, the electrons transferred to a dielectric surface can be released into a vacuum after contact electrification. Therefore, TENG cannot maintain an effective electrical output under high-temperature conditions. Here, a series of high-temperature operatable flexible TENGs (HO-TENGs) based on nanofiber/microsphere hybrid membranes (FSHMs) was fabricated by electrospinning and electrospraying. The V_oc of HO-TENG is 212 V, which is 2.33 times higher than that of control TENG. After 10,000 cycle stability tests, the HO-TENG shows excellent durability. Especially, this HO-TENG can maintain 77% electrical output at 70 °C compared to room temperature, showing excellent high-temperature operability. This study can not only provide a reference for the construction of advanced high-performance TENG, but also provide a certain experimental basis for efficient collection of mechanical energy in high-temperature environment and promote the application of TENG devices in harsh environments.

Heterogeneous electric field distributions, uneven Zn ²⁺ ion flux, and interfacial crosstalk typically trigger irreversible Zn redox reactions, accelerating the degradation of Zn‐metal energy storage systems. Herein, we present an interfacial stabilization strategy that addresses key challenges in Zn redox chemistry through the rational design of electrostatic potential gradients within cellulose‐based separators. The functionalization of cellulose nanofibrils (CNFs) with precisely arranged electron‐donating polyethyleneimine (PEI) and electron‐accepting benzimidazole moieties establishes a well‐defined bidirectional electron transfer network. PEI‐mediated electron donation to both the CNF matrix and benzimidazole ring stabilizes the surface charge environment via the interfacial dipole effect, while synergistic electron migration toward the π‐conjugated benzimidazole ring increases electron density at coordination‐active nitrogen sites, thereby enhancing Zn ²⁺ binding affinity. The strengthened Zn‐N interactions lower the desolvation energy barrier, accelerate Zn ²⁺ transport kinetics, and suppress parasitic interfacial reactions, collectively enabling homogeneous Zn deposition and improved interfacial stability. Consequently, the Zn||Zn symmetric cells exhibit exceptional reversibility over 600 h at 20 mA cm ⁻² and 20 mAh cm ⁻² . When paired with MnO ₂ cathode, the full pouch cell retains 85.8% of its capacity after 4000 cycles at ∼10 C. This work highlights that molecular functionalization of separators enables next‐generation aqueous Zn batteries.