Menghao Yang

Unlocking the recycling and application of spent zinc‐manganese dry batteries (SZMBs) can effectively unleash the potential of urban resources. A zinc‑ion electrolyte strategy is proposed herein, which directly employs recycled ZnO from SZMBs within a ternary deep eutectic solvent (DES) of choline chloride (ChCl), urea, and ethylene glycol (EG). Regulating EG amount renders the ZnO‐based electrolyte suitable for a wide temperature range. Spectroscopic and dynamics simulations reveal that EG weakens the energy barrier for Zn ²⁺ reduction, achieving reversible Zn ²⁺ /Zn ⁰ redox. Simultaneously, the DES adsorbed on the Zn anode induces a solid electrolyte interphase film for guiding preferential zinc deposition along the Zn(100) plane. The ZnO‐based electrolyte enables the Zn||Zn symmetric cell to operate steadily for over 4100 h at 25°C, over 200 h at 60°C, and over 1400 h at –10°C. The Zn||PANI full cell delivers a specific capacity of 220 mA h g ⁻¹ at 0.1 A g ⁻¹ and maintains a capacity retention of 93.98% after 175 cycles at 0.5 A g ⁻¹ . This integrated design concept not only provides a practical value‐added approach for the utilization of zinc from SZMBs, but also offers a feasible strategy for the development of new high‐performance, wide‐temperature zinc‐ion battery electrolytes.

Upcycling highly stable polytetrafluoroethylene (PTFE) waste into value‐added carbon materials is fundamentally hindered by its complete zero‐residue pyrolysis, which exclusively emits hazardous fluorocarbons rather than forming solid carbon frameworks. Herein, we present a scalable zeolite‐particle‐templated cocarbonization strategy that catalytically transforms industrial PTFE waste into hierarchical porous carbon nanosheets (PCNs) while fixing over 81% of the fluorine as recyclable NaF. Comprehensive mechanistic investigations reveal that the ZSM‐5 template electronically activates C─F bonds and lowers the defluorination barrier, driving a successive‐condensation structural evolution. The resulting PCN, featuring an ultrahigh specific surface area and hierarchical porosity, delivers exceptional dual‐mode energy storage performances. In supercapacitors, PCNs achieve a remarkable specific capacitance of 429.6 F g ⁻¹ and outstanding rate capabilities driven by reversible pseudocapacitance and ion coadsorption. Concurrently, in carbon‐based aqueous zinc‐ion batteries (CAZBs), the PCNs deliver a high specific capacity of 267.0 mAh g ⁻¹ with robust extreme‐temperature adaptability (−25°C). Validated by a continuous industrial‐scale piping and instrumentation design (PID), this strategy demonstrates high commercial viability with low energy storage costs, pioneering a waste‐to‐wealth strategy for advanced carbon materials for energy storage.

Upcycling highly stable polytetrafluoroethylene (PTFE) waste into value‐added carbon materials is fundamentally hindered by its complete zero‐residue pyrolysis, which exclusively emits hazardous fluorocarbons rather than forming solid carbon frameworks. Herein, we present a scalable zeolite‐particle‐templated cocarbonization strategy that catalytically transforms industrial PTFE waste into hierarchical porous carbon nanosheets (PCNs) while fixing over 81% of the fluorine as recyclable NaF. Comprehensive mechanistic investigations reveal that the ZSM‐5 template electronically activates C─F bonds and lowers the defluorination barrier, driving a successive‐condensation structural evolution. The resulting PCN, featuring an ultrahigh specific surface area and hierarchical porosity, delivers exceptional dual‐mode energy storage performances. In supercapacitors, PCNs achieve a remarkable specific capacitance of 429.6 F g ⁻¹ and outstanding rate capabilities driven by reversible pseudocapacitance and ion coadsorption. Concurrently, in carbon‐based aqueous zinc‐ion batteries (CAZBs), the PCNs deliver a high specific capacity of 267.0 mAh g ⁻¹ with robust extreme‐temperature adaptability (−25°C). Validated by a continuous industrial‐scale piping and instrumentation design (PID), this strategy demonstrates high commercial viability with low energy storage costs, pioneering a waste‐to‐wealth strategy for advanced carbon materials for energy storage.

Solid-state electrolytes (SSEs) are pivotal for next-generation energy systems, offering enhanced safety and higher energy density. In particular, a fundamental challenge in garnet-type Li7La3Zr2O12 (LLZO) and lithium superionic conductor Li10GeP2S12 (LGPS) applications is understanding and controlling the mechanical behavior at interfaces and under operational stresses, which can induce microcracking, void formation, and lithium dendrite growth. To address this gap, we employ machine learning interatomic potentials (MLIPs) with near-DFT accuracy and perform large-scale MD simulations to investigate two critical aspects: (1) the mechanical deformation of bulk LLZO under uniaxial compression and tension, revealing atomic-level mechanisms of elastic and plastic deformation, crack initiation, and failure; and (2) the kinetics of prescribed Li-atom insertion at model interfaces, exploring nucleation, clustering, and interface dynamics. Specifically, we identify two distinct lithium diffusion mechanisms: lithium ions in LGPS migrate via stepwise hopping along one-dimensional channels; in contrast, LLZO exhibits cooperative crowding (or “pushing”) within a three-dimensional network, where ion migration involves collective displacements and local structural distortions. These studies provide novel atomistic insights into the mechanical stability of SSEs under stress and the interfacial processes governing Li-atom insertion and clustering, contributing to the understanding and mitigation of key failure mechanisms in solid-state batteries.

Eliminating platinum group metals from cathode catalysts in low-temperature polymer electrolyte fuel cells is highly important for addressing the sustainability challenge fuel cell systems face. Here, we propose modifying the electronic structure of Li-intercalated layered Mn-oxide as a cathode catalyst to overcome the activity/stability tradeoff in anion exchange membrane fuel cells. To achieve this goal, we deploy a precious metal free catalyst design strategy involving atomically dispersed p -block metal Sn doped in Li ₂ MnO ₃ , in addition to d -block metals, which has been poorly explored in the research thus far. Operando X-ray absorption spectroscopy and rapid freeze-quench ¹¹⁹ Sn Mössbauer methodology are employed to visualize the catalytic dynamics, revealing that part of Mn ⁴⁺ ions are converted into Mn ³⁺ ions, whereas Sn ⁴⁺ ions remain unchanged during the oxygen reduction reaction. Under H ₂ /O ₂ conditions, anion exchange membrane fuel cells employing Li ₂ Mn _0.9 Sn _0.1 O ₃ cathodes achieve peak power densities above 1.0 W cm ^-2 _geo and 3.96 W mg ^-1 _Pt . This work demonstrates the beneficial modulation of the electronic structure through p -block metal substitution in earth-abundant Mn-enriched oxide materials.

Accurate prediction of ion transport properties remains a key bottleneck in computational discovery of solid‐state electrolytes, particularly because experimentally measured ionic conductivities are sparse and strongly dependent on crystal structure. Here we introduce USMNet, a unified structure‐aware multimodal neural network that combines crystal‐structure representations, compositional features, and physically motivated descriptors to predict lithium‐ion conductivity. We benchmark the model against composition‐only and structure‐based baselines, showing that explicit structural information improves prediction accuracy and enables data‐efficient and reliable exploration of candidate materials. We then apply USMNet to 168 675 candidate materials spanning 19 lithium solid‐state electrolyte frameworks, identifying 21 high‐potential inorganic electrolytes. Selected candidates are synthesized and experimentally validated, with Li ₁₆ ZnSiP ₂ S ₁₆ enabling all‐solid‐state batteries that retain 80% capacity after 600 cycles under 0.5 C at room temperature. These results establish a generalizable structure‐aware learning strategy for electrochemical property prediction and demonstrate its utility in accelerating closed‐loop materials discovery under limited data regimes.

Electrolyte leakage poses an urgent safety challenge to the development of the energy industry, and real‐time monitoring of such leakage enables early mitigation of potential hazards, including thermal runaway, fires, and battery explosions. Herein, a concept of “organic‐inorganic ion co‐conduction” was proposed to guide the in situ synthesis of porous organic‐inorganic hybrid ionic conductors on electrodes via a modular interface‐confined route, which enabled the simultaneous incorporation of “soft” ionic liquids and “hard” metal‐organic frameworks into a tailored porous conductive polymer substrate. Leveraging the abundant porosity and efficient ionic conductivity, the developed sensors exhibited excellent selectivity toward representative ether‐based and carbonate‐based electrolytes, demonstrating low detectable concentration, rapid response‐recovery time (2/3 s), low operating voltage (10 mV), and exceptional operational stability (>3 months). Interestingly, the sensor could detect a trace volume of commercial electrolytes (10 nL) within seconds and retained stable performance after 1000 bending cycles. Furthermore, it was integrated into a portable module that wirelessly transmits detection data to smartphones via Bluetooth. Density functional theory calculations further revealed that the unique sensing response arose from strong dual‐site ion‐dipole interactions. It offers a promising platform for early electrolyte leakage warning and other safety‐critical applications in next‐generation battery systems.

Owing to their vast crustal abundance and inherently dendrite‐free electrodeposition, rechargeable magnesium batteries (RMBs) have emerged as a compelling next‐generation alternative to conventional lithium‐ion technologies. In this context, Prussian Blue Analogs (PBAs) demonstrate significant potential as intercalation cathode candidates, as their open framework and continuous 3D diffusion pathways facilitate efficient divalent ion transport. However, their practical implementation is currently hindered by limited specific capacity and insufficient cycling stability, primarily due to lattice distortion and sluggish intercalation kinetics. This study presents a novel magnesium storage mechanism involving vacancy‐mediated ion insertion (4b sites) and the activation of adsorption‐active sites (32f sites), thereby significantly boosting the electrochemical performance of PBA materials. Notably, the cation‐deficient PBA (PBA□Fe), synthesized via slow coprecipitation and acid treatment, delivered a high energy density of 240 Wh kg ⁻¹ , which is comparable to those of transition metal oxide materials, while maintaining 80.7% capacity retention over 1000 cycles at 200 mA g ⁻¹ . The dual role of Fe vacancies—providing Mg ²⁺ storage sites and activating additional adsorption active sites (32f sites)—highlights a strategic innovation for the deployment of high‐capacity and long‐cycle cathodes for RMBs. This work underscores the potential of defect engineering in optimizing high‐performance Mg‐ion battery materials.

Bismuth‐based electrocatalysts have shown great promise for the electrochemical reduction of CO ₂ to formate. However, taming the active crystal facets to realize high selectivity and long‐term stability remains a fundamental challenge. Herein, we describe a facile one‐step electrodeposition strategy that enables the bismuth nanosheets to dominantly expose the (110) facet via deposition potential modulation. Particularly, the bismuth catalyst structure undergoes in operando reconstruction, in which the highly active (110) facet appears and is well maintained during the electrolysis owing to the reduction from Bi ³⁺ to metallic Bi ⁰ . Therefore, the bismuth catalyst with ultrathin nanosheets exhibits high catalytic activity and long‐term durability, achieving over 90% Faradaic efficiency for formate over a wide potential range from −0.7 to −1.3 V _RHE . When assembled in a Zn‐CO ₂ battery, the bismuth‐based cathode catalyst also demonstrates stable cycling, further confirming the robust durability of the (110)‐facet‐stabilized catalyst under operating conditions. Mechanistic studies reveal that the (110) facet facilitates the CO ₂ activation process and stabilizes the critical *OCHO intermediate, thereby promoting the reaction pathway selectively toward formate formation while suppressing the competitive hydrogen evolution reaction. This work establishes a facet‐engineering strategy via a facial electrochemical synthesis as the accessible route for designing high‐performance CO ₂ reduction reaction catalysts.