Zhipeng Ma

CeO ₂ ‐based electrocatalysts are promising for the oxygen evolution reaction (OER) owing to their distinctive Ce ³⁺ /Ce ⁴⁺ redox flexibility, large oxygen‐storage capacity, and lattice adaptability. More importantly, CeO ₂ can dynamically regulate catalyst surface reconstruction and electronic structure while significantly enhancing catalytic activity and long‐term stability. In this review, we first focus on CeO ₂ ‐based electrocatalysts for OER from structural characteristics, design principles and strategies, structure–property relationships, interfacial structure, as well as critical evaluation of design strategies and selection principles. The mechanistic roles of CeO ₂ in OER are highlighted, including redox chemistry and oxygen‐vacancy (O _v ) dynamics, electronic‐structure modulation and charge transfer, interfacial coupling and surface reconstruction, as well as operando evidence and the controversy over lattice‐oxygen participation. The performance of CeO ₂ ‐based OER electrocatalysts in different electrolytes, including alkaline, acidic, and seawater media, is also summarized to demonstrate their applicability under diverse operating conditions. Finally, from the perspectives of electronic‐structure evolution, redox‐state transitions, lattice evolution, and catalytic pathways, this review summarizes the underlying mechanisms by which CeO ₂ regulates the dynamic catalytic behavior of OER and provides an outlook on future design strategies for developing highly efficient and durable CeO ₂ ‐based electrocatalysts.

The self‐corrosion of zinc anodes, caused by zinc atom escape and hydrogen evolution, remains a fundamental obstacle to the deployment of aqueous zinc‐ion batteries (AZIBs) in sustainable energy storage systems. Herein, we develop a scalable Cr(III) passivation strategy that constructs an ultrathin (∼100 nm), dense Cr ₂ O ₃ layer on the zinc surface, delivering the highest zinc chemical potential (6.96 eV) among various commercial passivation materials. This design establishes a steep chemical potential gradient, significantly elevating the energy barrier for zinc escape and thereby mitigating self‐corrosion under resting conditions. Moreover, strong electrostatic interactions between Cr ₂ O ₃ and [Zn(H ₂ O) ₆ ] ²⁺ accelerate Zn ²⁺ desolvation and migration, guiding zinc to deposit beneath the passivation layer while eliminating interference from solvated water molecules. Benefiting from its ability to inhibit static corrosion and stabilize the electrode interface during cycling, the electrode achieves remarkably stable operation over 7300 h. Furthermore, full‐cell integration with commercial MnO ₂ shows negligible capacity fading over 200 cycles in a 1 Ah hard‐shell battery, and an unprecedented device energy density of 45 Wh kg ⁻¹ is achieved at an ultrahigh capacity up to ∼4 Ah. This work establishes an effective interfacial design that alleviates resting‐state corrosion and enhances cycling stability for promoting the practical application of AZIBs.

The spin‐state engineering of transition‐metal catalysts plays a decisive role in enhancing electrocatalytic activity in lithium‐sulfur batteries. While high/low‐spin transitions are accessible for 3 d ⁴ ‐3 d ⁷ ions in octahedral fields, Ni ²⁺ (3 d ⁸ ) has long been considered spin‐inert under such coordination. Herein, we demonstrate that ferromagnetic NiF ₂ effectively circumvents this limitation through exchange‐mediated spin alignment. In contrast to antiferromagnetic NiO, the parallel spin ordering in NiF ₂ generates a permanent magnetic moment and upshifts the d‐band center, thereby promoting the injection of spin‐polarized electrons into the antibonding π* orbital of S─S bonds in lithium polysulfides. This strong d‐π coupling significantly reduces the S─S bond order and facilitates sulfur reaction kinetics. As a result, Li‐S batteries with the NiF ₂ catalyst deliver an initial capacity of 842.7 mAh g ⁻¹ at 1 C and exhibit exceptional cycling stability, with a capacity increase to 941.6 mAh g ⁻¹ after 500 cycles. Moreover, a high areal capacity of 7.2 mAh cm ⁻² is achieved under elevated sulfur loading (8 mg cm ⁻² ). This work breaks the conventional spin blockade in Ni ²⁺ catalysts and offers a strategic approach to spin‐level electrocatalyst design for efficient sulfur redox reactions.

From the perspective of cross-scale collaborative design, this review systematically summarizes the multi-dimensional modification strategies for copper foil current collectors in anode-free lithium metal batteries (AFLMBs).

Zinc (Zn) metal, with abundant resources, intrinsic safety, and environmental benignity, presents an attractive prospect as a novel electrode material. However, many substantial challenges remain in realizing the widespread application of aqueous Zn‐ion batteries (AZIBs) technologies. These encompass significant material corrosion challenges (This can lead to battery failure in an unloaded state.), hydrogen evolution reactions, pronounced dendrite growth at the anode interface, and a constrained electrochemical stability window. Consequently, these factors contribute to diminished battery lifespan and energy efficiency while restricting high‐voltage performance. Although numerous reviews have addressed the potential of electrode and separator design to mitigate these issues to some extent, the inherent reactivity of water remains the fundamental source of these challenges, underscoring the necessity for precise regulation of active water molecules within the electrolyte. In this review, the failure mechanism of AZIBs (unloaded and in charge and discharge state) is analyzed, and the optimization strategy and working principle of water in the electrolyte are reviewed, aiming to provide insights for effectively controlling the corrosion process and hydrogen evolution reaction, further controlling dendrite formation, and expanding the range of electrochemical stability. Furthermore, it outlines the challenges to promote its practical application and future development pathways.

Currently, the realization of controllable Li electrodeposits to further extend the cycling life of Li metal anode remains challenging. Herein, it is reported that carbon nanosheet array‐loaded ferromagnetic CoF₂ nanoparticles on carbon cloth (CC@CoF₂/C) as an internal micro‐magnetic field source to manipulate the dynamic trajectory of Li⁺ deposition via the magnetohydrodynamic effect. This approach ensures uniform lithium‐ion distribution and improves deep plating capacity, achieving a prolonged cycle life of the dendrite‐free Li anode. Finite element simulations, in situ characterizations, and electrochemical tests confirm that magnetic CoF₂ not only guides Li⁺ migration through Lorentz force to prevent dendritic growth but also improves uniform Li deposition due to the in situ conversion of LiF‐rich solid electrolyte interphase during electroplating. Meanwhile, a CC@CoF₂/C‐based half‐cell operates stably over 10 000 h at 1 mA cm⁻² with a low 7.8 mV overpotential. When matched with a commercial LiFePO₄ cathode, the full cell reveals a high capacity of 122.96 mAh g⁻¹ at a 2 C rate after 1000 cycles, retaining 91.95% capacity. The proposed strategy can be effectively expanded and adapted to investigate the deposition behavior of a wide range of metal anodes, offering a versatile and robust analytical framework for addressing diverse metal‐based electrochemical systems.

Rechargeable aqueous batteries adopting Fe-based materials are attracting widespread attention by virtue of high-safety and low-cost. However, the present Fe-based anodes suffer from low electronic/ionic conductivity and unsatisfactory comprehensive performance, which greatly restrict their practicability. Concerning the principle of physical chemistry, fabricating electrodes that could simultaneously achieve ideal thermodynamics and fast kinetics is a promising issue. Herein, hierarchical Fe₃O₄@Fe foam electrode with enhanced interface/grain boundary engineering is fabricated through an in situ self-regulated strategy. The electrode achieves ultrahigh areal capacity of 31.45 mA h cm^-2 (50 mA cm^-2), good scale application potential (742.54 mA h for 25 cm² electrode), satisfied antifluctuation capability, and excellent cycling stability. In/ex situ characterizations further validate the desired thermodynamic and kinetic properties of the electrode endowed with accurate interface regulation, which accounts for salient electrochemical reversibility in a two-stage phase transition and slight energy loss. This work offers a suitable strategy in designing high-performance Fe-based electrodes with comprehensive inherent characteristics for high-safety large-scale energy storage.