An overview of self-discharge mechanisms in supercapacitors, including physicochemical insights, mitigation strategies, and emerging concepts aimed at enhancing energy retention and device longevity.

Abstract The in‐depth understanding of local atomic environment–property relationships of p‐block metal single‐atom catalysts toward the 2 e − oxygen reduction reaction (ORR) has rarely been reported. Here, guided by first‐principles calculations, we develop a heteroatom‐modified In‐based metal–organic framework‐assisted approach to accurately synthesize an optimal catalyst, in which single In atoms are anchored by combined N,S‐dual first coordination and B second coordination supported by the hollow carbon rods (In SAs/NSBC). The In SAs/NSBC catalyst exhibits a high H 2 O 2 selectivity of above 95 % in a wide range of pH. Furthermore, the In SAs/NSBC‐modified natural air diffusion electrode exhibits an unprecedented production rate of 6.49 mol peroxide g catalyst −1 h −1 in 0.1 M KOH electrolyte and 6.71 mol peroxide g catalyst −1 h −1 in 0.1 M PBS electrolyte. This strategy enables the design of next‐generation high‐performance single‐atom materials, and provides practical guidance for H 2 O 2 electrosynthesis.

The development of clean and efficient renewable energy is of great strategic importance to realize green energy conversion and low-carbon growth. Hydrogen energy, as a renewable energy with "zero carbon emission", can be efficiently converted into hydrogen energy and electric energy by electrolysis of water to hydrogen technology. Anion-exchange membrane water electrolysis (AEMWE), substantially advanced by nonprecious metal electrocatalysts, is among the most cost-effective and promising water electrolysis technologies, combining the advantages of proton exchange membranes with the proven technology of traditional alkaline water electrolysis and potentially eliminating the disadvantages of both. In this paper, the latest results of AEMWE research in recent years are summarized, including the AEMWE mechanism study and the hot issues of low-cost transition metal hydrogen evolution reaction and oxygen evolution reaction electrocatalyst design in recent years. The key factors affecting the performance of AEMWE are pointed out, and further challenges and opportunities encountered in large-scale industrialization are discussed. Finally, this review provides strong guidance for advancing AEMWE.

Abstract The in‐depth understanding of local atomic environment–property relationships of p‐block metal single‐atom catalysts toward the 2 e − oxygen reduction reaction (ORR) has rarely been reported. Here, guided by first‐principles calculations, we develop a heteroatom‐modified In‐based metal–organic framework‐assisted approach to accurately synthesize an optimal catalyst, in which single In atoms are anchored by combined N,S‐dual first coordination and B second coordination supported by the hollow carbon rods (In SAs/NSBC). The In SAs/NSBC catalyst exhibits a high H 2 O 2 selectivity of above 95 % in a wide range of pH. Furthermore, the In SAs/NSBC‐modified natural air diffusion electrode exhibits an unprecedented production rate of 6.49 mol peroxide g catalyst −1 h −1 in 0.1 M KOH electrolyte and 6.71 mol peroxide g catalyst −1 h −1 in 0.1 M PBS electrolyte. This strategy enables the design of next‐generation high‐performance single‐atom materials, and provides practical guidance for H 2 O 2 electrosynthesis.

Abstract Elucidating the synergistic catalytic mechanism between multiple active centers is of great significance for heterogeneous catalysis; however, finding the corresponding experimental evidence remains challenging owing to the complexity of catalyst structures and interface environment. Here we construct an asymmetric TeN 2 –CuN 3 double-atomic site catalyst, which is analyzed via full-range synchrotron pair distribution function. In electrochemical CO 2 reduction, the catalyst features a synergistic mechanism with the double-atomic site activating two key molecules: operando spectroscopy confirms that the Te center activates CO 2 , and the Cu center helps to dissociate H 2 O. The experimental and theoretical results reveal that the TeN 2 –CuN 3 could cooperatively lower the energy barriers for the rate-determining step, promoting proton transfer kinetics. Therefore, the TeN 2 –CuN 3 displays a broad potential range with high CO selectivity, improved kinetics and good stability. This work presents synthesis and characterization strategies for double-atomic site catalysts, and experimentally unveils the underpinning mechanism of synergistic catalysis.

Metal ion substitution and anion exchange are two effective strategies for regulating the electronic and geometric structure of spinel. However, the optimal location of foreign metallic cations and the exact role of these metals and anions remain elusive. Herein, CoFe2O4-based hollow nanospheres with outstanding oxygen evolution reaction activity are prepared by Cr3+ substitution and S2– exchange. X-ray absorption spectra and theoretical calculations reveal that Cr3+ can be precisely doped into octahedral (Oh) Fe sites and simultaneously induce Co vacancy, which can activate adjacent tetrahedral (Td) Fe3+. Furthermore, S2– exchange results in structure distortion of Td-Fe due to compressive strain effect. The change in the local geometry of Td-Fe causes the *OOH intermediate to deviate from the y-axis plane, thus enhancing the adsorption of the *OOH. The Co vacancy and S2– exchange can adjust the geometric and electronic structure of Td-Fe, thus activating the inert Td-Fe and improving the electrochemical performance.

Abstract The fabrication of heterostructures has inspired extensive interest in promoting the performance of solar cells or solar fuel production, but it is still challenging for nitrides to prepare structurally ordered heterostructures. Herein, one nickel nitride‐based heterostructure composed of 1D Ni 0.2 Mo 0.8 N nanorods and 0D Ni 3 N nanoparticles (denoted as NiMoN/NiN) is reported to exhibit significantly promoted hydrogen evolution reaction performance in both alkaline and neutral media. In particular, the optimal overpotential of the NiMoN/NiN sample at 10 mA cm −2 in 1 m KOH is 49 mV. The successful fabrication of 1D/0D heterostructures is mainly ascribed to morphology‐inherited nitridation of 1D oxide precursor (denoted as NiMoO‐NRs) in situ grown on Ni foam surface, and attributed to strong Lewis acid–base interaction that renders the Ni 2+ ions emitted from the oxide precursor to well coordinate with NH 3 for the formation of Ni 3 N nanoparticles during the nitridation process. It is theoretically and experimentally demonstrated that the special 1D/0D heterostructure provides tandem active phases Ni 0.2 Mo 0.8 N and Ni 3 N for synergistic promotion in lowering the activation energy of H 2 O dissociation and optimizing the adsorption energy of H, respectively. This work may open a new avenue for developing highly active tandem electrocatalysts for promising renewable energy conversion.

Highly efficient La/Sr-based perovskites with surface Fe sites and Sr vacancies were developed for the active lattice oxygen mechanism (LOM) of the oxygen evolution reaction (OER), and a relationship between the LOM and dynamic surface structure was established.

Abstract Complex metal nanoparticles distributed uniformly on supports demonstrate distinctive physicochemical properties and thus attract a wide attention for applications. The commonly used wet chemistry methods display limitations to achieve the nanoparticle structure design and uniform dispersion simultaneously. Solid-phase synthesis serves as an interesting strategy which can achieve the fabrication of complex metal nanoparticles on supports. Herein, the solid-phase synthesis strategy is developed to precisely synthesize uniformly distributed CoFe@FeO x core@shell nanoparticles. Fe atoms are preferentially exsolved from CoFe alloy bulk to the surface and then be carburized into a Fe x C shell under thermal syngas atmosphere, subsequently the formed Fe x C shell is passivated by air, obtaining CoFe@FeO x with a CoFe alloy core and a FeO x shell. This strategy is universal for the synthesis of MFe@FeO x (M = Co, Ni, Mn). The CoFe@FeO x exhibits bifunctional effect on regulating polysulfides as the separator coating layer for Li-S and Na-S batteries. This method could be developed into solid-phase synthetic systems to construct well distributed complex metal nanoparticles.

Sluggish surface reaction is a critical factor that strongly governs the efficiency of photocatalytic solar fuel production, particularly in CO 2 -to-ethanol photoconversion. Here, inspired by the principles underlying enzyme catalytic proficiency and specificity, we report a biomimetic photocatalyst that affords superior CO 2 -to-ethanol photoreduction efficiency (5.5 millimoles gram −1 hour −1 in average with 98.2% selectivity) distinctly surpassing the state of the art. The key is to create a class of catalytic pocket, which contains spatially organized NH 2 …Cu-Se(-Zn) multiple functionalities at close range, over ZnSe colloidal quantum wells. Such structure offers a platform to mimic the concerted cooperation between the active site and surrounding secondary/outer coordination spheres in enzyme catalysis. This is manifested by the chemical adsorption and activation of CO 2 via a bent geometry, favorable stabilization toward a variety of important intermediates, promotion of multielectron/proton transfer processes, etc. These results highlight the potential of incorporating enzyme-like features into the design of photocatalysts to overcome the challenges in CO 2 reduction.

Dietary deficiencies in essential micronutrients and other phytonutrients represent a global health and economic burden, contributing to “hidden hunger” and chronic diseases. While genome editing has been employed to improve individual nutritional traits in crops, multibiofortification through simultaneous modification of multiple distinct metabolic pathways is more challenging. Here, we designed a multiplex CRISPR-Cas strategy to edit five key genes in tomato: Sl7-DR2 , SlGAD3 , SlSGR1 , SlGGP1 , and SlGGP2 . This approach successfully generated quintuple mutant ( 5m ) tomato lines simultaneously biofortified with seven health-promoting compounds: vitamin D 3 (from 0 to 0.70 μg/g dry weight), vitamin C (up to 2.53-fold), provitamin A/β-carotene (up to 3.86-fold), α-carotene (up to 2.47-fold), lutein (up to 3.26-fold), lycopene (up to 7.07-fold), and γ-aminobutyric acid (GABA, up to 5.26-fold). Notably, these multibiofortified tomatoes exhibited no significant trade-offs in plant growth or fruit quality. Extracts from 5m tomatoes showed enhanced suppression of colorectal cancer cell proliferation in vitro. This antiproliferative effect was validated in vivo, where dietary supplementation with 5m tomato powder significantly inhibited tumor growth in a mouse xenograft model. Our work demonstrates an effective strategy for developing a next generation of “functional foods” through multibiofortification, creating a single, nutrient-dense crop that combats both micronutrient malnutrition and chronic diseases.

Abstract Single‐atom nanozymes (SAzymes) can effectively mimic the metal active centers of natural enzymes at the atomic level owing to their atomically dispersed active sites, thereby maximizing atom utilization efficiency and density of active sites. Hence, SAzymes can be considered the most promising candidates to replace natural enzymes. Herein, a PEGylated mesoporous Mn‐based single‐atom nanozyme (PmMn/SAE) employing a coordination‐assisted polymerization pyrolysis strategy that uses polydopamine for photothermal‐augmented nanocatalytic therapy is designed. PmMn/SAE exhibits excellent multiple enzymatic performance, including catalase‐like, oxidase‐like, and peroxidase (POD)‐like performance, due to the atomically dispersed Mn active species. As a result, PmMn/SAE not only catalyzes the decomposition of endogenous H 2 O 2 to generate O 2 for relieving hypoxia inside the tumor but also transfers electrons to O 2 to produce superoxide radicals to kill tumor cells. Meanwhile, PmMn/SAE is able to trigger Fenton‐like reactions to generate highly toxic hydroxyl radicals to induce cancer cell apoptosis. The POD‐like catalytic mechanism of mMn/SAE is revealed using experimental results and density functional theory. Furthermor, PmMn/SAE shows good photothermal conversion efficiency (η = 22.1%) in the second near‐infrared region (1064 nm). Both the in vitro and in vivo experimental results indicate that PmMn/SAE can effectively kill cancer cells through photothermal‐enhanced catalytic therapy.

ABSTRACT Data‐driven artificial intelligence provides strong technical support for addressing global energy and environmental issues. The powerful data processing and analysis capabilities of machine learning (ML) can quickly predict electrocatalytic performance, improving the efficiency of catalyst design and addressing the time‐consuming and inefficient nature of traditional catalyst design. By integrating ML with theoretical calculations and experiments, catalytic reaction processes can be precisely regulated. This not only accelerates the discovery of new catalysts but also drives the development of more efficient and environmentally friendly sustainable energy technologies. In this article, we discuss new approaches to discovering novel catalysts driven by ML, focusing on catalytic activity prediction, reaction energy barrier optimization, and the design of innovative catalytic materials. We systematically analysis the application of ML in the field of electrocatalysis and explore the future prospects of ML in this domain. We provide a comprehensive and in‐depth analysis of the application of ML in the field of electrocatalysis and explore its potential for future development.