Wenjun Zhang

Simultaneously achieving fast kinetics and interfacial stability remains a formidable challenge for quasi-solid-state zinc-iodine batteries. Herein, we introduce the interfacial kosmotropic effect via a low-cost CaSO ₄ ·2H ₂ O ionic matrix to actively reconstruct the interfacial chemistry. Through the precise regulation of the electrical double layer, the strong electrostatic fields from surface-bound kosmotropic ions organize limited water molecules into a low-activity, confined network, fundamentally reshaping the solvation structure. Benefiting from this optimized atomic-level architecture, the reaction pathways are fundamentally altered: on the cathode, it unlocks a single-step I ⁻ /I ₂ redox process that effectively severs the formation pathway of polyiodides; on the anode, it induces coordinatively unsaturated structures to accelerate desolvation and suppress parasitic reactions. Consequently, the system circumvents intrinsic kinetic limitations and facilitates a transition from electric-field-driven electromigration to regulated diffusion-dominated transport. This optimizes ion flux and enables stable Zn anode operation for >1000 h (99.7% avg. Coulombic efficiency). The Zn-I ₂ full cells deliver a high areal capacity of 0.91 mAh cm ⁻² with 93% capacity retention after 2500 cycles at 1.0 mA cm ⁻² . Impressively, this strategy enables a minimalist iodine-free cathode design and successfully scales to pouch cells (stable for >600 cycles), offering a paradigm shift for developing safe, high-rate and durable quasi-solid-state batteries.

High‐voltage (>4.3 V) Ni‐rich layered cathodes are central to high‐energy‐density lithium‐ion batteries, yet their practical operation is limited by coupled mechanical degradation, sluggish interfacial charge transport, and parasitic cathode‐electrolyte reactions. Herein, we report a slurry‐compatible strategy to construct a phase‐separated mosaic‐like interphase on LiNi _0.8 Co _0.1 Mn _0.1 O ₂ (NCM811) cathodes using poly(acrylonitrile‐styrene‐acrylate) (ASA) as a multifunctional additive. During N‐methyl‐2‐pyrrolidone (NMP)‐based slurry casting and electrode drying process, the core‐shell ASA precursor undergoes structural reorganization, forming an ASA‐derived interphase composed of poly (butyl acrylate) (PBA)‐rich elastomeric regions and poly(styrene‐co‐acrylonitrile) (SAN)‐rich polar/aromatic regions. The PBA‐rich component buffers volume‐change‐induced stress and suppresses particle cracking, while the SAN‐rich component contributes to Li ⁺ ‐related interfacial affinity and enhances electron conductive. This phase‐separated, mosaic‐like interphase promotes stress dissipation from intercalation (deintercalation), enabling simultaneous regulation of mechanical integrity, interfacial chemistry, and electrode kinetics. Consequently, the optimized cathode exhibits reduced polarization, enhanced Li ⁺ diffusion, suppressed transition‐metal dissolution, and stabilized electrode interphases. In practical NCM811||graphite pouch cells under 4.5 V operation, capacity retention increases from 55.2% to 78.7% after 500 cycles, increased by 43%. This strategy highlights the importance of regulating the phase organization of polymeric slurry additives, offering a practically compatible route for stabilizing high‐voltage layered oxide cathodes.

The development of efficient and durable electrocatalysts for industrial-level water splitting remains a critical challenge. Here we report a CuO-MoS2/MoO3 precatalyst that undergoes electrochemical reconstruction under working conditions to yield two distinct active phases: Cu-MoS2 for the hydrogen evolution reaction (HER) at the cathode and an optimized CuO-MoS2/MoO3 for the oxygen evolution reaction (OER) at the anode. In 1.0 M KOH, the reconstructed electrodes deliver remarkably low overpotentials of 35 mV for HER and 124 mV for OER at 10 mA cm-2, along with outstanding long-term durability, sustaining 500 mA cm-2 for 100 h. Combined in situ Fourier-transform infrared spectroscopy and density functional theory calculations reveal that Cu species not only enhance charge transport but also tailor the electronic structure to optimize intermediate adsorption and reorganize interfacial water into a strongly hydrogen-bonded network, thereby accelerating water dissociation and proton transfer kinetics. When assembled into an anion-exchange-membrane water electrolyzer, the system delivers 1.0 A cm-2 at a low voltage of 1.77 V and 80 °C, with stable operation for 500 h, substantially surpassing noble-metal benchmarks. Our findings offer an efficient and durable catalyst system for sustainable hydrogen production, as well as fundamental insights into catalyst reconstruction and interfacial water regulation that inform the rational design of electrocatalytic materials.

Electrocatalytic nitrate reduction reaction (NO ₃ RR) towards ammonia (NH ₃ ) production is a critical process that sustainably converts hazardous nitrate to value‐added chemicals. Amorphous metal‐based nanomaterials are promising NO ₃ RR catalysts owing to the abundant surface active sites, but their performance is still unsatisfactory for practical needs. We develop a robust one‐pot strategy to prepare a family of amorphous PdMP ( a ‐PdMP, M = Cu, Ni, Co, Fe, Mn, and Zn) nanoparticles with high yield, high structural stability, uniform morphology, and tunable composition. Impressively, the as‐prepared a ‐PdCoP nanoparticles show excellent electrocatalytic activity (onset potential measured at +0.3 V vs. reversed hydrogen electrode), high NH ₃ selectivity, and outstanding long‐term stability (Faradaic efficiency (FE) maintained > ∼98% at 200 mA cm ⁻² for 200 h) in NO ₃ RR. Theoretical calculations demonstrate that alloying in PdM can enhance overall electron exchange/transfer, while phosphization helps to stabilize the metal valence. Particularly, the a ‐PdCoP possesses a moderate d‐band center to avoid intermediate overbinding, meanwhile, it has the lowest work function to accelerate the electron transfer during NO ₃ RR. Our work demonstrates that synergistic amorphization and phosphization of Pd alloy nanocatalysts can greatly promote their activity and durability in NO ₃ RR. The universal synthesis approach provides guidance to prepare amorphous multielement nanomaterials as highly efficient electrocatalysts.

The developed Lewis acidic molecular additive enables synchronous anion immobilization and decomposition, yielding a stable SEI layer, effective cation–anion decoupling, and accelerated Zn ²⁺ transport kinetics.

Electrochemical nitrate (NO ₃ ⁻ ) reduction presents a multifunctional strategy to remediate NO ₃ ⁻ contamination while enabling ammonia (NH ₃ ) synthesis. However, it is still a challenge to achieve satisfied performance due to the multiple rate‐limiting steps and competitive hydrogen evolution, particularly under neutral conditions and low concentrations. Herein, a set of single‐atom catalysts (SACs) featuring high loading of multiple metal sites was synthesized as tandem catalysts for NO ₃ ⁻ to NH ₃ . Fe/Cu/Pd−N−C SACs exhibit a superior performance with the high NH ₃ Faradaic efficiency of 98%, 95%, and 82% at the NO ₃ ⁻ concentration of 0.5, 0.1, and 0.01 M , respectively, which are much higher than these of other SACs. Moreover, it also performed very well in the stability and anti‐interference measurements. The exceptional performance is proved to be attributable to the tandem interplay among Fe, Cu, and Pd sites. Specifically, NO ₃ ⁻ undergoes reduction to NO ₂ ⁻ over Cu single atoms, and NO ₂ ⁻ then migrates to Fe single atoms for the subsequent conversion, benefiting from the high adsorption energy. Meanwhile, Pd sites can regulate the generation rate and consumption pathway of active hydrogen. This work offers a viable solution for the recycling and utilization of nitrate pollutants and provides a flexible design strategy for multifunctional electrocatalysts.

Conventional rechargeable zinc-air batteries (ZABs) face two critical challenges: (1) slow kinetics of the oxygen reduction (ORR) and oxygen evolution (OER) reactions; and (2) the thermodynamic incompatibility of OER and ORR occurring concurrently on a single air cathode. To address these limitations, we propose in this study a dual-cathode zinc-ethylene glycol/air battery (D-ZEAB) that spatially decouples ORR and the ethylene glycol oxidation reaction (EGOR) onto separate cathodes, enabling concurrent electricity generation and electroreforming of polyethylene terephthalate (PET) plastic waste into high-value C₂ chemicals. Furthermore, we develop a bifunctional catalyst composed of defect-rich subnanometer-thick PdCuCo trimetallenes to enhance both EGOR and ORR kinetics. Benefiting from the decoupled cathode configuration and the bifunctional PdCuCo catalyst, the D-ZEAB demonstrates an energy conversion efficiency of 91.7%, a long cycle life of 1696 h, and a Faradaic efficiency of >93% for GA production. This work not only presents a promising strategy for advancing the zinc-air battery technology but also offers a sustainable route for simultaneous energy storage and plastic waste upcycling.