http://onlinelibrary.wiley.com/rss/journal/10.1002/(ISSN)1521-4095

This work designs a macromolecular ordering-tuned interphase by leveraging the phase-separated hierarchical ion tunnels in semicrystalline polymers to address Zn/electrolyte interfacial issues. The PVA interphase, with lamellar orientation parallel to the Zn anode, achieves a balance between electrode protection and ionic conductivity, enabling rapid yet uniform Zn2+ transport and interfacial stability.

The energy density and cycle life of aqueous zinc metal batteries are hindered by inherent chemical and mechanical instabilities at the Zn/electrolyte interface, causing uncontrolled dendrite formation and side reactions. Here, an anisotropic crystalline polymer interphase by leveraging the hierarchical structure to stabilize the interface is designed. The stabilization effect strongly depends on the crystallinity of polymer chains, where the one with optimal ion transfer possesses a preferred orientation of nanocrystals parallel to the Zn anode. This topological structure creates fast tunnel for ion transport that significantly enhances the kinetics and reversibility of electrochemical transformations. The ordered crystalline phase and disordered amorphous phase respectively blocks H₂O penetration and provides Zn2⁺ transport channels, reaching an optimum between electrode protection and ion transfer. Symmetric cells with the crystallinity-tuned interface demonstrate an exceptionally long lifespan exceeding 3000 h at elevated current density and capacity of 5 mA cm−2 and 5 mAh cm−2, with a cumulative plated capacity of 7500 mAh cm−2. The Zn/AC hybrid ion supercapacitor exhibits outstanding stability, enduring over 10 000 cycles at 5 A g−1. The work unveils new ordering-dependent ion transport in solid-state polymer interphase/electrolyte and provides a feasible approach for advancing grid-scale aqueous batteries.

Featuring low energy consumption and easy integration with modern electronic, electrocaloric polymer is a highly promising alternative to vapor-compression systems. Here, the synergistic electro-thermal phase change methodology boosted the performance of electrocaloric materials, achieving a dramatic temperature drop in simulated electronic chip cooling. This methodology opened up a new way for enhancing the entropy change of electrocaloric materials.

Electro-phase change materials (electro-PCM), based on the electrocaloric effect, have attracted significant attention and achieved rapid development in the field of cooling technology owing to their environmental protection, low energy consumption, and miniaturization. However, due to their limited isothermal entropy change and thermal conductivity, the cooling capacity of the electro-PCM devices has severely limited their cooling effect on electronic devices. Here, with the synergistic electro-thermal phase changes, the entropy change and thermal conductivity of electro-PCM are significantly improved by stacking it with thermo-phase change materials (thermo-PCM). Compared with that of the electro-PCM, the entropy change and thermal conductivity of electro-thermal phase change materials (ETPCM) stack can be up to 4.68-fold (from 28.31 to 132.35 J kg−1 K−1 at electric field of 100 MV m−1) and 2.39-fold (from 0.18 to 0.43 W m−1·K−1), respectively. The practicality of this strategy has also been fully validated by cooling a simulated electronic chip (1.75 W cm−2) with a temperature drop of 49.32 K after constructing ETPCM stack-based cooling device using the electrostatic actuation prototype. The synergistic enhancement of entropy change and thermal conductivity paves the way for the future direction of electrocaloric cooling toward interdisciplinary fusion.

Strategic embedding of 3D norbornene units in fused-ring acceptors suppresses excessive aggregation, synergistically boosting photoluminescence quantum yield (PLQY) and achieving a record-breaking power conversion efficiency (PCE) of 20.4% and an extremely low voltage loss (V loss) of 0.548 V in organic solar cells.

This study outlines a molecular design approach that entails integrating 3D structural motifs into the central core or terminal groups of fused-ring acceptor molecules, specifically, LLZ1, LLZ2, and LLZ3–by incorporating a 3D architecture unit of norbornene. The objective is to modulate the aggregation behavior of these molecules by modifying their molecular structure, thereby enhancing the photoluminescence quantum yield (PLQY) values of the acceptor materials and reducing the non-radiative recombination voltage loss in the corresponding devices. Our research findings demonstrate that the introduction of norbornene units effectively suppresses excessive molecular aggregation and significantly improves the PLQY values of the acceptor molecules. Further research has demonstrated that only the acceptor molecule LLZ1, characterized by both high PLQY and moderate crystallinity, can strike an optimal balance between the dual requirements of reducing voltage loss and enhancing charge transport in the device. Utilizing the preferred molecule LLZ1, we achieved a power conversion efficiency (PCE) of 18.0% in binary system and 20.4% in ternary device with much-reduced voltage loss of 0.508V, which is among the highest values of current OSCs. In summary, this work provides novel insights and research directions for the development of OSCs with low voltage loss and high PCE.

Relying on the porous nacre-like framework, large-scale thermal-protective ceramic is produced via a simple bottom-up film-to-bulk assembly strategy. This porous ceramic achieves the combination of mechanical and anisotropic thermal properties, making it good candidate for complex thermal protection applications.

Ever more severe energy dilemma and unfulfilled demands for thermal protection applications have drawn a great interest in developing thermal protective materials. Though great progress is achieved by implementing several advanced micro-architectures, the conflict between thermal insulation and mechanical properties, along with the complex manufacturing process, remains the main obstacles for fabricating ideal integrated thermal insulation materials. Here, a scalable nacre-like porous ceramic is reported with a good combination of thermal insulation and mechanical strength (≈0.058 W m−1 K−1, 22 MPa) via a bottom-up film-to-bulk assembly. The well-aligned microplatelets constructed the nacre-like framework and produced porosity in between for thermal insulation while the mineral bridges between microplatelets connected and strengthened the whole framework. Besides, the structure-induced anisotropy of thermal conductivity on out-plane and in-plane directions provides the possibilities for heat management. Moreover, this material shows an excellent fire-resistance and maintained performance after fire. These structure-induced integrated superiorities made this material good candidate for complex thermal protection applications.

The LiNiO2@LiFePO4 composite material with coherent combination exhibits remarkable cyclability, rate capability and high first-cycle Coulombic efficiency. The coherent oriented channels favor the reversible and rapid lithium-ion transport with suppressed strain accumulation while phosphate anions anchored on the LiNiO2 surface stabilizes Ni sites, mitigating surface degradation.

LiNiO2 is an appealing cathode material for Li-ion batteries because of high energy density and low cost but suffers from irreversible phase transition and surface instability. Herein, a ball-milled LiNiO2@LiFePO4 composite with oriented coherent combination is reported with enhanced structural stability and Li+ diffusion. The coherent oriented channels are demonstrated to favor the reversible and rapid Li+ intercalation during the H2-H3 phase transition, which significantly alleviates structural strain accumulation. The covalent P─O bonds anchored on the LiNiO2 surface stabilizes the Ni sites, mitigating surface reconstruction and lattice oxygen loss. The LiNiO2@LiFePO4 cathode exhibits a specific capacity of 210 mAh g−1 and an initial Coulombic efficiency of 93.7% at 0.1 C, along with a remarkable rate capability of 156 mAh g−1 at 10 C. Furthermore, the full cells pairing LiNiO2@LiFePO4 cathode and graphite anode deliver a considerable energy density over 280 Wh kg−1 and a remarkable capacity retention. This study offers an effective approach of phosphate coalesce to upgrade high-capacity nickel-rich oxide cathode materials.

By exploiting the layered nature of GeSe, the carrier transport direction is effectively restrict, resulting in giant spin lifetimes. This leads to efficient spin injection at room temperature and gate tunable spin transport at low temperatures. Additionally, the results suggest that GeSe is the only air-stable 2D semiconductor suitable for spin transport channels at room temperature.

The 2D materials are promising channel materials for spin transistors due to their natural spatial-confined carrier transport character. Nonetheless, electrical spin injection and detection in 2D semiconductors used to be challenging. This study reports high-efficient spin injection and transport in 2D GeSe, which exhibits moderate spin-orbit coupling (SOC) and extended spin diffusion lengths due to the van der Waals structure. The non-local magnetoresistance (MR) measurements show a maximum spin polarization of 18.31%, a long spin diffusion length of 255.98 nm, and a giant spin relaxation time of 17.6 ns at room-temperature. After cooling to 4.3 K, the elevated spin diffusion length further increases to 397.04 nm, with an elevated spin polarization of 25.38%, leading to the successful observation of local MR in a two-terminal lateral spin valve. Additionally, the spin transport characteristics are also tunable by gate voltages due to the field-dependent SOC and Rashba spin relaxation. This study highlights GeSe as an air-stable 2D semiconductor with anisotropic and gate-tunable spin transport capability. The results will remove the barriers to developing novel spintronic devices based on emerging 2D semiconductors.

The mechanoluminescence microcilia array film with a bionic hair-like structure achieves an ultralow activation threshold of just 10 mN—the lowest reported to date—enabled by stress concentration. With excellent sensitivity to dynamic mechanical stimuli, mechanoluminescence-derived texture discrimination and Braille recognition with high accuracy is demonstrated for the first time via integration with an image-based machine learning approach.

Mechanoluminescence (ML)-based sensing technology opens up new opportunities for photonic/electronic skin due to their self-powered nature, visible spatial mapping of mechanical stimuli, and intrinsic responses to dynamic forces. However, challenges such as weak brightness and high activation threshold have hindered their development. Inspired by hair-like structures of human skin, skin-bionic mechanoluminescent PDMS/ZnS:Cu microcilia array film (MLMCA) is fabricated using a magnetic field-assisted template method. The MLMCA exhibits tunable aspect ratios and ML intensity, with the underlying relationship between microcilia structure and ML performance clarified through finite element analysis. The MLMCA achieves an ultralow activation threshold at the micronewton level (≈10 mN) owing to the stress concentration induced by high aspect ratio. With excellent sensitivity to dynamic mechanical stimuli, the MLMCA enables texture recognition with an accuracy of 99.95% when integrated with the image machine learning approach. Furthermore, an ML-based Braille-to-speech translation system is developed and achieved a high recognition accuracy of 96.74%. This study not only tackles the persistent limitation of high activation thresholds in ML-based sensing but also pioneers the practical use of ML-based tactile sensing in texture discrimination and Braille reading.