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

High-performance ultrathin (≈7.8 µm) polycarbonate-based electrolyte (UPCE) is fabricated, without the use of additional liquid additives. The designed UPCE delivers a high ionic conductivity (4.8 × 10−4 S cm−1) and an ultrahigh critical current density (11.5 mA cm−2) at 25 °C. The 4.5 V solid-state Li|LiCoO2 cell demonstrates an ultralong lifespan cycling stability over 1500 cycles at 1 C.

Ultrathin solid-polymer-electrolytes (SPEs) are the most promising alternative substituting for the conventional liquid electrolyte to enable high-energy-density, safe lithium-metal-batteries (LMBs). Nevertheless, developing ultrathin SPEs with both high ionic conductivity, and strong Li dendrite retardant is still a significant challenge. Here a scalable fabrication of high-performance ultrathin (≈7.8 µm) polycarbonate-based electrolyte (UPCE) is proposed via electrolyte structural engineering, phase separation-derived poly(vinylidene fluoride-co-hexafluoropropylene) (PVH) porous scaffold, without use of additional liquid additives. The rational electrolyte structural modulation with 1-fluoro-4-(1-methylethenyl)benzene (FMB) enables a weakened Li+-polymer interaction due to weak Li+ solvation with fluorine, benzene ring, facilitates the formation of LiF-rich solid-electrolyte-interphase on Li metal surface. As a result, the designed UPCE delivers a high ionic conductivity of 4.8 × 10−4 S cm−1, an ultrahigh critical current density of 11.5 mA cm−2 at 25 °C. The solid-state Li symmetric cell attains unprecedented ultralong cycling over 6000 h at 0.5 mA cm−2. Furthermore, the Li|LiCoO2 cell cycles stably over 1500 cycles at a high operating voltage of 4.5 V, and the pouch cell can achieve a high energy density of 495 Wh kg−1 excluding the packaging. This work offers a new pathway inspiring efforts to commercialize ultrathin SPEs for high-energy solid-state LMBs.

This study designs modular oligomeric donors (5BDD, 5BDD-F, 5BDT-F, 5BDT-Cl) for ternary OSCs, achieving PCEs >20%. By systematically tuning energy levels, we reveal material compatibility, not HOMO alignment, drive V OC enhancement, suppress ACQ and reduce energy loss, offering new design principles for high-efficiency OSCs.

In organic solar cells (OSCs), the ternary strategy is a mainstream approach to obtaining highly efficient OSCs. A deeper understanding of working mechanisms and the material selection criteria for boosting open-circuit voltage (V OC) is essential for further OSC breakthrough. Through a modular design principle, a series of oligomeric donors – 5BDD, 5BDD-F, 5BDT-F, and 5BDT-Cl – with similar molecular configurations but varying HOMO levels is systematically designed. These findings reveal that the HOMO levels of these oligomers have a negligible impact on the V OC of the ternary OSCs. Instead, their excellent compatibility with acceptors played a pivotal role in enhancing V OC. The oligomers effectively suppressed excessive acceptor aggregation and achieved Aggregation-Caused Quenching Suppression (ACQS), strengthening the external electroluminescence quantum efficiency (EQEEL) and reducing non-radiative recombination energy losses. Simultaneously, oligomers fine-tuned and optimized the morphology of the blend films, leading to a higher fill factor (FF) and improved performance. Notably, the 5BDT-F- and 5BDT-Cl-based ternary OSCs achieved impressive power conversion efficiencies (PCEs) of 19.8% and 20.1% (certified 19.76%), with FFs of 80.9% and 80.7%, respectively. This work elucidates the unusual role of the third component energy levels on the V OC in ternary OSCs and offers valuable guidance for future OSC design.

A photo-activated Co/Cu dual-atom catalyst on C₃N₄ is developed to construct dynamic catalytic domains, enabling accelerated sulfur redox kinetics and uniform Li₂S deposition. This strategy delivers outstanding rate capability and long-term stability in lithium-sulfur batteries under high-loading and lean-electrolyte conditions, offering new insights into light-driven electrocatalyst engineering.

Lithium-sulfur batteries (LSBs) face significant challenges due to sluggish reaction kinetics and the polysulfide shuttle effect. Here, a light-induced anchoring strategy is employed to construct Co/Cu diatomic catalysts (DACs) on C3N4, introducing dual active sites with strong polysulfide adsorption and bifunctional catalytic activity. Upon light excitation, the synergistic Co–Cu interaction induces local electronic redistribution, which triggers broader electronic rearrangement and directional charge carrier migration. This process generates dynamic catalytic domains with enhanced polysulfide adsorption and catalytic conversion capability. These domains not only promote effective photogenerated carrier separation but also play a pivotal role in accelerating sulfur redox kinetics and regulating Li₂S deposition behavior. As a result, the Co/Cu-C₃N₄ cathode exhibits exceptional electrochemical performance, achieving 1200 stable cycles at 8 C with a capacity decay of 0.025% per cycle. Remarkably, under lean electrolyte conditions (E/S = 4 µL mg⁻¹) and ultra-high sulfur loading (14.73 mg cm⁻2), the battery maintains excellent cycling stability. This work offers a conceptual framework for photo-induced catalytic microenvironment design and highlights the potential of spatiotemporal electronic modulation for next-generation photo-assisted energy storage systems.

Introducing a Mg interlayer at the junction simultaneously stabilizes Mg3(Bi,Sb)2 materials and contacts for over 100 days. This dual stabilization derives from suppressing detrimental Mg diffusion and compensating for Mg loss, thereby maintaining an outstanding power density of 0.45 W cm−2 and remarkable conversion efficiency of 8.6% in aged modules, offering new insights for durable thermoelectric energy harvesting.

Thermoelectric technology offers a promising pathway toward global sustainability by harvesting waste heat. However, long-term stability is hindered by inevitable elemental diffusion, degrading both the thermoelectric junction and material properties, which prevents the realization of power generation applications. Here, dual and superior stability is achieved in high-performance Mg3(Bi,Sb)2, surpassing prior studies that focus on either junction or material stability. By introducing an Mg layer at the junction, detrimental Mg diffusion is suppressed and compensate for Mg loss in the material, effectively stabilizing both junctions and materials for over 100 days. As a result, a thermoelectric module with 30-day-aged Mg3(Bi,Sb)2 is able to maintain an outstanding power density of 0.45 W cm−2 and remarkable conversion efficiency of 8.6%, demonstrating unprecedented stability. These findings provide new insights into thermoelectric junction engineering, shifting from interface optimization to comprehensive stabilization, advancing the practical viability of thermoelectric energy harvesting for renewable and waste heat applications.

This work proposes a dual sites activation strategy to enhance the nucleophilic of Sn sites and modulate the Cu sites as harder Lewis acid sites by constructing CuS/SnS2 Mott–Schottky catalysts. The optimized charge distribution facilitates the adsorption of CO2 and *OCHO intermediates simultaneously, thus improving formic acid selectivity in acid electrolytes under industrial current densities.

Electroreduction of CO2 to formic acid in acidic media offers a promising approach for value-added CO2 utilization. However, achieving high selectivity for formic acid in acidic electrolytes remains challenging due to the competitive hydrogen evolution reaction (HER), particularly at industrially relevant current densities. Herein, a charge redistribution modulation strategy is demonstrated by constructing the CuS /SnS2 Mott–Schottky catalyst to enhance formic acid selectivity. Experiments and calculation results reveal the broadening of Sn orbitals and reduced orbital symmetry of Sn orbitals contribute to enhanced CO2 adsorption, while the modulated Cu sites with a stronger Lewis acid character stabilize *OCHO intermediates more effectively. This enables dual-site activation for efficient CO2 electroreduction into formic acid synthesis. Consequently, the optimized CuS/SnS2 catalysts achieve a maximum formic acid Faradaic efficiency (FE) of 99% in acidic electrolytes and maintain selectivity above 80% at a current density of 1 A cm−2, significantly surpassing the performance of CuS and SnS2 alone. Moreover, the excellent selectivity across pH-universal electrolytes demonstrates that dual-site activation is a promising strategy for designing highly efficient CO2 reduction reaction catalysts.

Ultrathin amorphous CoO nanosheets are synthesized via a low-temperature annealing strategy. Amorphization induces modulated energy levels and an increased population of unpaired electrons in the frontier d-orbitals of Co atoms. These features enhance the 3d yz –2px interactions between the Co center and the C atom in the CO2 molecule, thereby facilitating its adsorption and activation compared to crystalline CoO.

Photocatalytic CO2 conversion into syngas presents a sustainable avenue for mitigating carbon emissions while generating value-added fuels. However, sluggish charge carrier dynamics and weak, non-specific interactions between catalytic sites and CO2 molecules limit efficiency. Herein, ultrathin amorphous CoO nanosheets (a-CoO) are reported that integrate structural and electronic advantages for enhanced CO₂ photoreduction. X-ray absorption spectroscopy and density functional theory analyses reveal that amorphization partially transforms the local crystal field of Co from quasi-octahedral to quasi-tetrahedral coordination, resulting in a greater population of unpaired electrons in the frontier d-orbitals. This reconfiguration promotes electron injection from Co 3dyz into the 2π* antibonding orbitals component of C 2px in CO2, which strengthens 3d-2p orbital hybridization and lowers the activation energy barrier. In situ spectroscopic further confirms that this orbital restructuring accelerates charge transfer from the Co center to CO2 and facilitates its activation. Meanwhile, the ultrathin 2D architecture improves the separation and transport of photoexcited carriers. Consequently, vigorous bubbles are observed under visible light irradiation, with a total syngas evolution rate of 23.7 mmol g−1 h−1 (12.6 and 11.1 mmol g−1 h−1 for CO and H2, respectively) and an apparent quantum efficiency of 1.28% at 450 nm—≈8.7-fold improvement over its crystalline counterpart.