Tao Yang

This review elucidates the operating microenvironment, function, and regulation strategies of anodic ionomers, highlighting how interfacial interactions and multi-mass transport govern efficient and durable membrane water electrolysis.

Spin‐state modulation has emerged as an effective strategy to overcome the sluggish spin‐forbidden transition from singlet H ₂ O to triplet O ₂ , thereby improving the oxygen evolution reaction (OER) performance. Perovskite oxides provide an excellent platform for spin regulation owing to their structural stability, rich active sites, and wide range of controllable electronic states. This review provides a comprehensive overview of perovskite oxide structures and their classification. It then elucidates the principles of spin‐state regulation and their significance for OER. The spin‐related mechanisms behind distinct OER pathways are illustrated, alongside state‐of‐the‐art spin characterization and analytical techniques. The strategies of doping, defect engineering, and lattice strain engineering for tuning the spin state to boost the OER activity of perovskite oxides are summarized. Finally, the remaining challenges associated with spin modulation and the prospects for future development are critically discussed.

Charge accumulation has significant impacts on the activity and stability of oxygen evolution reaction (OER) catalysts, especially under high current density conditions. However, the formation mechanisms of charge accumulation and its mechanism on OER catalyst performance remain unclear. There is a lack of a mechanism for guiding the design of OER catalyst structure‐performance from the perspective of regulating charge accumulation. Therefore, herein the formation mechanisms of charge accumulation in OER catalysts are revealed. Charge accumulation composition and its influence on the activity and stability of OER catalysts, as well as the corresponding boundary conditions, are systematically summarized. Based on this, directional and controllable regulation mechanisms are elucidated from the two perspectives of “charge accumulation in the low‐potential range promoting OER catalyst activity” and “charge accumulation in the high‐potential range undermining OER catalyst stability”. Specifically, charge accumulation under low current density is promoted by increasing double‐layer capacitance, deprotonation capacitance, and pseudocapacitance. Conversely, charge accumulation under high current density is suppressed through strategies such as doping, intercalation engineering, and heterojunction construction. This review provides theoretical design guidance for developing high‐performance OER catalysts for industrial‐scale current densities.

Electrochemical water splitting has emerged as a sustainable paradigm for hydrogen generation, where sluggish kinetics of the oxygen evolution reaction (OER) catalyzed by transition metal‐based materials remain the critical bottleneck. Herein, we present a strategy that anchors CeO _x nanoparticles (∼2 nm) onto two‐dimensional Ni(OH) ₂ nanosheets, enabling dual modulation of spatial configuration and electronic states to accelerate O–O coupling. Spatially, interfacial lattice distortion between CeO _x and Ni(OH) ₂ optimizes Ni–Ni dual‐metal sites with reduced interatomic spacing. Electronically, dynamic modulation through reversible Ce ³⁺ /Ce ⁴⁺ redox cycling positions Ce as an electronic regulation hub, stabilizing Ni species at the catalytically favorable +3 oxidation state through Ce─O─Ni interactions. This synergistic effect shifts the pathway from adsorbate evolution mechanism (AEM) to oxide pathway mechanism (OPM). The prepared CeO _x @Ni(OH) ₂ achieves an overpotential of 152 mV at 10 mA cm ⁻² and operates continuously over 2000 h with limited performance decay. When integrated into an alkaline anion exchange membrane water electrolyzer (AEMWE), it requires 1.91 V to attain 1 A cm ⁻² and maintains stable operation for 450 h. This OPM activation strategy shows potential applicability across CeO _x ‐loaded transition metal hydroxides, including Ni(OH) ₂ , Co(OH) ₂ , NiCo, and NiFe layered double hydroxides, offering a promising approach for alkaline OER enhancement.

Electrochemical water splitting has emerged as a sustainable paradigm for hydrogen generation, where sluggish kinetics of the oxygen evolution reaction (OER) catalyzed by transition metal‐based materials remain the critical bottleneck. Herein, we present a strategy that anchors CeO _x nanoparticles (∼2 nm) onto two‐dimensional Ni(OH) ₂ nanosheets, enabling dual modulation of spatial configuration and electronic states to accelerate O–O coupling. Spatially, interfacial lattice distortion between CeO _x and Ni(OH) ₂ optimizes Ni–Ni dual‐metal sites with reduced interatomic spacing. Electronically, dynamic modulation through reversible Ce ³⁺ /Ce ⁴⁺ redox cycling positions Ce as an electronic regulation hub, stabilizing Ni species at the catalytically favorable +3 oxidation state through Ce─O─Ni interactions. This synergistic effect shifts the pathway from adsorbate evolution mechanism (AEM) to oxide pathway mechanism (OPM). The prepared CeO _x @Ni(OH) ₂ achieves an overpotential of 152 mV at 10 mA cm ⁻² and operates continuously over 2000 h with limited performance decay. When integrated into an alkaline anion exchange membrane water electrolyzer (AEMWE), it requires 1.91 V to attain 1 A cm ⁻² and maintains stable operation for 450 h. This OPM activation strategy shows potential applicability across CeO _x ‐loaded transition metal hydroxides, including Ni(OH) ₂ , Co(OH) ₂ , NiCo, and NiFe layered double hydroxides, offering a promising approach for alkaline OER enhancement.

The surface chemistry of MXenes is a central factor governing electrochemical performance and has become increasingly complex with the emergence of molten salt etching routes. Compared with conventional fluoride‐derived systems, molten salt derived MXenes exhibit chemically diverse and highly tunable surface states arising from termination chemistry, retained metal species, interfacial evolution, and post‐synthetic regulation. Such synthesis‐dependent complexity creates a strongly coupled design space that motivates data‐driven discovery. In this review, we summarize recent progress in molten salt derived MXenes with emphasis on tunable surface chemistry and its implications for data‐driven design. Surface termination engineering, metal incorporation, heterostructure formation, and post‐synthetic modification are discussed as interconnected surface‐regulation pathways. We further examine how synthesis history, surface chemistry, and electronic structure can be translated into physically meaningful descriptors for machine learning and high‐throughput modeling. Overall, this review establishes a chemistry‐informed framework linking molten salt synthesis, tunable surface chemistry, and data‐driven discovery toward electrochemical applications.

Aqueous zinc–iodine (Zn–I ₂ ) batteries have demonstrated remarkable potential in extensive energy storage. Nevertheless, the practical application of Zn–I ₂ batteries is constrained by the shuttle effect of polyiodide species. To address this issue, two hydrazone‐linked two‐dimensional (2D) covalent organic frameworks (COFs), named Por‐AQ‐COF and Por‐BT‐COF, were prepared under solvothermal conditions. Powder X‐ray diffraction, N ₂ adsorption isotherm, and electron microscopy tests reveal the 2D tetrahedral structure geometry of both COFs with one‐dimensional (1D) channels. In particular, the abundant hydrazone groups in the channels of both COFs lead to their excellent Zn ²⁺ adsorption capacity, promoting their adsorption and activation of polyiodide species. This endows both Por‐AQ‐COF and Por‐BT‐COF with excellent Zn–I ₂ batteries performance, achieving a capacity of 871 mA h g ⁻¹ at 2 A g ⁻¹ (corresponding to an energy density of 1045 W h kg ⁻¹ ), outstanding rate capability (554 mA h g ⁻¹ retained at 10 A g ⁻¹ with an energy density of 643 W h kg ⁻¹ ), and excellent cycling stability, surpass all previously reported host materials used in iodine electrode of Zn–I ₂ batteries. This research would provide new insight into the design of porous host materials to inhibit the shuttle effect of polyiodide species for Zn–I ₂ batteries with high performance and stability.

Accurate simulation of strongly correlated electron systems is a major challenge for designing clean and efficient energy materials. Density functional theory (DFT) is widely used for electronic structure calculations, but it fails for systems with localized d or f orbital electrons because it neglects dynamic electron-electron correlations. The DFT + U method, rooted in the Hubbard model, overcomes this limitation by balancing computational efficiency and accuracy. Its predictive power strongly depends on the correct choice of the Hubbard U parameter. This review first explains the theoretical basis of the Hubbard model and the DFT + U framework. It then systematically describes U determination techniques, including experimental fitting, linear response methods and their derivatives, pseudo hybrid functional approaches, and machine learning enabled optimization strategies. We compare their computational merits and applicability. Finally, we discuss emerging paradigms, such as combining first principles screening with adaptive machine learning workflows. These advances promise to improve the precision and scalability of strongly correlated system modeling and accelerate the rational design of next generation energy materials.