Dong Su

High-nickel single-crystal cathodes effectively address the poor mechanical stability and severe side reactions that plague their polycrystalline counterparts. However, they introduce new structural challenges, including extended Li+ diffusion pathways, which in turn lead to structural slips, lattice distortions, and phase transformations, ultimately compromising both electrochemical capacity and structural stability. Herein, we report a state-of-the-art cathode architecture for high-nickel materials, derived from high-energy neutron irradiation of single-crystal LiNi0.92Co0.06Mn0.02O2 particles. This process induces long-range Li/Ni antisite disorder and short-range metal–oxygen octahedral distortions, concurrently yielding a nanostructure of abundant grain boundaries and interwoven layered/rock-salt nanodomains within the single-crystalline particles. These grain boundaries are proposed to constitute a 3D percolation network for rapid Li+ transport, whereas the interwoven nanodomains may act as local structural reinforcing units that help suppress irreversible phase transitions and the propagation of interfacial side reactions during cycling. These characteristics are favorable for sustaining continuous Li+ deintercalation/intercalation and reversible electrochemistry, thereby preserving the structural stability of the single-crystal framework while simultaneously shortening diffusion pathways. As a result, the engineered cathode delivers a high specific discharge capacity of 213.9 mAh/g at 0.2 C and 152.2 mAh/g at 10 C (within 4.5 V). Moreover, it retains 80.0% of its initial capacity after 450 cycles at 5 C, significantly outperforming the reference single-crystal cathode (64.2%). This work establishes high-energy neutron irradiation as an effective cathode reconstruction strategy, offering a viable route toward robust, high-energy cathodes.

Efficient recycling and high‐value regeneration of spent LiCoO ₂ (LCO) cathodes are important for advancing lithium‐ion batteries (LIBs) recycling and promoting the sustainable utilization of critical resources. Here, we identify the intrinsic factors limiting the structural recovery of spent LCO (SLCO) and demonstrate that lattice reconstruction effectively restores both structural integrity and electrochemical stability at high voltages up to 4.6 V. We develop a multistep regeneration strategy that integrates selective impurity removal, lithium compensation, and high‐temperature solid‐state sintering to reconstruct the layered lattice and enhance Li ⁺ diffusion kinetics. Moreover, a uniform nanoscopic rock‐salt surface layer is deliberately engineered to suppress phase transitions and mitigate parasitic side reactions during high‐voltage cycling. Benefiting from these synergistic modifications, the regenerated LCO delivers good cycling stability, retaining 81.0% of its capacity after 1500 cycles at 2 C/4 C and achieving 121.3 mAh g ⁻¹ at 10 C under 4.6 V. This work provides a practical and scalable approach for regenerating SLCO cathodes with high‐voltage capability, offering new insights into green recycling and the sustainable development of LIBs cathode materials.

Boron nitride (BN) aerogels are highly attractive for thermal insulation systems by virtue of their ultra-low density and exceptional thermal insulation performance; yet, their practical application is severely limited by inadequate load-bearing capacity and insufficient ablation resistance. In this study, a large-scale polymer-derived silicon boron carbonitride (SiBCN)-reinforced BN hybrid aerogel (SiBCN/BN) was fabricated via impregnation, solvothermal treatment, and pyrolysis; critically, the SiBCN aerogels construct a mesoporous network within the macropores of the BN nanoribbon skeleton. The density (0.073–0.236 g·cm–3) and the micromorphology of the SiBCN/BN hybrid aerogels can be tuned by adjusting the SiBCN loading. The hierarchical pore structure endows the SiBCN/BN aerogel with low thermal conductivity at room temperature (0.042 W·m–1·K–1) and at high temperature (0.061 W m–1 K–1 @ 800 °C and 0.080 W m–1 K–1 @ 1000 °C). Notably, the SiBCN/BN hybrid aerogel exhibits enhanced compressive strength (1.36 MPa, 405-fold higher than that of the BN aerogel) and improved ablation resistance (only 1% linear shrinkage after 1000 °C ablation). These superior properties are attributable to the reinforcement and protective effects imparted by the SiBCN phase. Furthermore, the SiBCN/BN hybrid aerogel shows super-hydrophobicity with a water contact angle up to 150.6°, endowing it with self-cleaning and moisture-resistant properties. The synergistic enhancement in mechanical strength and thermal stability makes the SiBCN/BN hybrid aerogel an exceptional choice for lightweight thermal insulation, expanding its practical utility and paving the way for next-generation multifunctional, robust, and durable aerogel systems.

Lithium‐rich manganese‐based materials (LRM) are promising high‐energy cathodes with the ability to undergo anionic redox for higher capacity, whose potential is unfortunately challenged by the associated stability issues related to oxygen release. Herein, we demonstrate the possibility to improve the electrochemical stability of LRM through a facile gas‐induced surface reconstruction (GSR) strategy involving a direct sintering of a mixture of LRM and artificial graphite (AG). We identify that the emergence of a CO ₂ atmosphere during this heating treatment triggered the transition of the surface lattices from a layer‐typed feature into well‐regulated domains dominated by rock‐salt‐like structures, thereby effectively suppressing the activity of surface oxygen to combat the notorious interfacial side reactions. This surface‐engineered cathode exhibited improved cycling performance to achieve a capacity retention of 93.1% after 150 cycles when tested at 0.5 C as compared to only 65.8% for the untreated sample. Meanwhile, a suppressed voltage decay from 3.6 mV per cycle for the unmodified material to only 2.2 mV per cycle was observed. Our study highlights the critical role of surface chemistry in improving structural and electrochemical stability, and offering insights into surface lattice reconstruction to enhance the practical viability of high‐energy lithium‐ion batteries.

The spin polarization plays a critical role in heterogeneous catalysis by influencing the properties of active sites and thereby altering catalytic performance. However, precise construction of active sites with well-tuned spin states remains challenging. Here we demonstrate to manipulate the spin polarization of ferromagnetic cobalt (Co) centers in nitride catalysts by regulating the oxide mixology of precursors. The oxide mixology modulated the interaction between CoO_x and MoO₃ from local interfacial bonding to remote contacting. Strong and weak interactions induce the generations of Co₃Mo₃N and Co/γ-Mo₂N phases with low-spin and high-spin polarized Co centers, respectively, and Co centers with weakened spin polarization can facilitate the ammonia synthesis catalytic performance. Through the theoretical verification, we demonstrate that the spin-quenching configuration mitigates exchange splitting of Co centers, enabling efficient d-π* back-donation and enhancing N₂ activation. These findings open new perspectives for understanding the spin effect in heterogeneous catalysis and constructing well-defined spintronic catalysts.

Developing advanced iridium (Ir)–based oxygen evolution reaction (OER) catalysts is critical for proton exchange membrane water electrolyzers (PEMWEs). Unfortunately, conventional adsorbate evolution mechanism (AEM) and lattice oxygen mechanism (LOM) pathways suffer from an activity-stability trade-off, posing substantial challenges for catalyst design. Here, we report a charge-redistribution-induced oxygen (O) spillover strategy by designing amorphous VO _x -supported iridium-tin (IrSn) alloy OER catalysts, which can effectively transfer the poisoning oxygenated intermediates and maintain Ir valence stability (+2.5) during the dynamic OER to enhance activity and stability. In particular, the IrSn-VO _x –based PEMWE anode can deliver a current density of 3.0 amperes per square centimeter @ 1.798 volts (0.4 milligrams of platinum and Ir per square centimeter), surpassing the US Department of Energy (DOE) 2026 targets. A 25–square centimeter PEMWE operates stably for 5000 hours at industrial currents (≥25 amperes) with an exceptionally low degradation rate of 5.6 microvolts per hour, representing one of the best OER catalysts reported for practical PEMWEs. Theoretical calculations predict that the charge redistribution within IrSn-VO _x could reduce the kinetic energy barrier for *O spillover (from Ir to VO _x ) by 69% relative to O-O coupling, thus triggering the O spillover against the Ir overoxidation/dissolution. Consequently, IrSn–VO _x follows a support-involved LOM pathway with a reduced rate-determining-step barrier (0.37 electron volts) relative to IrSn following AEM (0.66 electron volts). In addition, Sn doping in IrSn-VO _x can further promote the regeneration of VO _x lattice O and improve stability.