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Abstract Near‐infrared (NIR) light powdered CO2 photoreduction reaction is generally restricted to the separation efficiency of photogenerated carriers and the supply of active hydrogen (*H). Herein, the study reports a retrofitting hydrogenated MoO3‐x (H‐MoO3‐x) nanosheet photocatalysts with Ru single atom substitution (Ru@H‐MoO3‐x) fabricated by one‐step solvothermal method. Experiments together with theoretical calculations demonstrate that the synergistic effect of Ru substitution and oxygen vacancy can not only inhibit the recombination of photogenerated carriers, but also facilitate the CO2 adsorption/activation as well as the supply of *H. Compared with H‐MoO3‐x, the Ru@H‐MoO3‐x exhibit more favorable formation of *CHO in the process of *CO conversion due to the fast *H generation on electron‐rich Ru sites and transfer to *CO intermediates, leading to the preferential photoreduction of CO2 to CH4 with high selectivity. The optimized Ru@H‐MoO3‐x exhibits a superior CO2 photoreduction activity with CH4 evolution rate of 111.6 and 39.0 µmol gcatalyst−1 under full spectrum and NIR light irradiation, respectively, which is 8.8 and 15.0 times much higher than that of H‐MoO3‐x. This work provides an in‐depth understanding at the atomic level on the design of NIR responsive photocatalyst for achieving the goal of carbon neutrality.

Abstract Simultaneously achieving high‐energy‐density and high‐power‐density is a crucial yet challenging objective in the pursuit of commercialized power batteries. In this study, atomic layer deposition (ALD) is employed combined with a coordinated thermal treatment strategy to construct a densely packed, electron‐ion dual conductor (EIC) protective coating on the surface of commercial LiNi0.5Co0.2Mn0.3O2 (NCM523) cathode material, further enhanced by gradient Al doping (Al@EIC‐NCM523). The ultra‐thin EIC effectively suppresses side reactions, thereby enhancing the stability of the cathode‐electrolyte interphase (CEI) at high‐voltages. The EIC's dual conduction capability provides a potent driving force for Li+ transport at the interface, promoting the formation of rapid ion deintercalation pathways within the Al@EIC‐NCM523 bulk phase. Moreover, the strategic gradient doping of Al serves to anchor the atomic spacing of Ni and O within the structure of Al@EIC‐NCM523, curbing irreversible phase transitions at high‐voltages and preserving the integrity of its layered structure. Remarkably, Al@EIC‐NCM523 displays an unprecedented rate capability (114.7 mAh g−1 at 20 C), and a sustained cycling performance (capacity retention of 74.72% after 800 cycles at 10 C) at 4.6 V. These findings demonstrate that the proposed EIC and doping strategy holds a significant promise for developing high‐energy‐density and high‐power‐density lithium‐ion batteries (LIBs).

Abstract Hydrogen (H2) has been regarded as a promising alternative to fossil‐fuel energy. Green H2 produced via water electrolysis (WE) powered by renewable energy could achieve a zero‐carbon footprint. Considerable attention has been focused on developing highly active catalysts to facilitate the reaction kinetics and improve the energy efficiency of WE. However, the stability of the electrocatalysts hampers the commercial viability of WE. Few studies have elucidated the origin of catalyst degradation. In this review, we first discuss the WE mechanism, including anodic oxygen evolution reaction (OER) and cathodic hydrogen evolution reaction (HER). Then, we provide strategies used to enhance the stability of electrocatalysts. After that, the deactivation mechanisms of the typical commercialized HER and OER catalysts, including Pt, Ni, RuO2, and IrO2, are summarized. Finally, the influence of fluctuating energy on catalyst degradation is highlighted and in situ characterization methodologies for understanding the dynamic deactivation processes are described.

Summary: Aqueous zinc-ion batteries (AZIBs) have garnered considerable interest as potential solutions for large-scale energy storage systems, owing to their cost-effectiveness and high safety. Nonetheless, the development of AZIBs is hindered by significant challenges associated with dendrite growth and side reactions on Zn anodes. Here, a bio-based separator derived from cellulose was developed for the dendrite-free anode in AZIBs. In addition, the separator is notable for its ultra-low cost and biodegradability in contrast to the commonly used commercial glass fiber (GF) separators. The mechanical strength of the separator is enhanced by the cross-linking of hydrogen bonds, effectively inhibiting dendrite growth. The zinc-philic groups facilitate better binding to Zn2+, resulting in uniform nucleation and deposition. The hydrophilic groups aid in trapping water molecules, thereby preventing side reactions of the electrolyte. The Zn||Zn symmetric cell with this separator can sustain a long cycle life for over 800 h, indicating stable Zn2+ plating and stripping with suppressed dendrite growth. Concurrently, the assembled Zn||VO2 full batteries exhibited a capacity retention rate of 61.87% after 1,000 cycles at 1 A g−1 with an initial capacity of 140 mAh g−1. This work highlights a stable, economical, and eco-friendly approach to the design of bio-based separators in AZIBs for sustainable energy storage systems.

Abstract Graphitic carbon nitride (g‐C3N4) is a highly recognized two‐dimensional semiconductor material known for its exceptional chemical and physical stability, environmental friendliness, and pollution‐free advantages. These remarkable properties have sparked extensive research in the field of energy storage. This review paper presents the latest advances in the utilization of g‐C3N4 in various energy storage technologies, including lithium‐ion batteries, lithium‐sulfur batteries, sodium‐ion batteries, potassium‐ion batteries, and supercapacitors. One of the key strengths of g‐C3N4 lies in its simple preparation process along with the ease of optimizing its material structure. It possesses abundant amino and Lewis basic groups, as well as a high density of nitrogen, enabling efficient charge transfer and electrolyte solution penetration. Moreover, the graphite‐like layered structure and the presence of large π bonds in g‐C3N4 contribute to its versatility in preparing multifunctional materials with different dimensions, element and group doping, and conjugated systems. These characteristics open up possibilities for expanding its application in energy storage devices. This article comprehensively reviews the research progress on g‐C3N4 in energy storage and highlights its potential for future applications in this field. By exploring the advantages and unique features of g‐C3N4, this paper provides valuable insights into harnessing the full potential of this material for energy storage applications.

Abstract Due to γ‐Bi2MoO6 (BMO) has attracted considerable attention because of its unique layered perovskite structure and excellent electrical conductivity. However, the easy recombination of electron–hole pairs limits its practical application. To address this issue, we successfully prepared aliovalent Cd2+ doped BMO (Cd‐BMO) by using a simple hydrothermal method for the degradation of the sulfamethoxazole (SMZ) and Rhodamine B (RhB). The result found that the degradation efficiency of Cd‐BMO is significantly higher than that of BMO, despite an increase in the bandgap after the introduction of Cd2+. The superior degradation efficiency of 8% Cd‐BMO, with a smaller particle size and larger specific surface area, can be attributed to its fast charge separation efficiency, low charge transfer resistance, and low rate of electron–hole pair recombination. Repeated and ion spillover experiments prove that 8% Cd‐BMO shows good stability and environmental protection. Theoretical simulation demonstrates that Cd offers electrons to the BMO system due to the decreased binding energy of BMO. The 8% Cd‐BMO sample can provide a suitable electric band edge for generating dominant active radicals during degradation. This work not only provides a potential candidate of 8% Cd‐BMO for practical degradation but also sheds light on the design of superior photocatalysts.

Highlights The mechanisms of the surface modification and structure design of zinc anode current collectors were summarized. The recent advances of high-performance zinc anode current collectors were reviewed and categorized according to their working mechanisms. The possible prospects and directions of zinc anode research were discussed.

Abstract Metal–sulfur battery, which provides considerable high energy density at a low cost, is an appealing energy‐storage technology for future long‐range electric vehicles and large‐scale power grids. One major challenge of metal–sulfur batteries is their long‐term cycling stability, which is significantly deteriorated by the generation of various soluble polysulfide intermediates and the shuttling of these intermediates through the separator. Furthermore, the intrinsically sluggish reaction kinetics associated with the poor conductivity of sulfur/sulfides family causes a large polarization in cycle behavior, which further deteriorates the electrode rechargeability. To solve these problems, the research communities have spent a great amount of effort on designing smart cathodes to delicately tailor the physiochemical interaction between the sulfur hosts and polysulfides. Here, we summarize the key progress in the development of two‐dimensional (2D) host materials showing advantageous tunability of their physiochemical properties through coordination control methods such as defect engineering, heteroatom doping, heterostructure, and phase and interface engineering. Accordingly, we discuss the mechanisms of polysulfide anchoring and catalyzing upon specific coordination environment in conjunction with possible structure–property relationships and theoretical analysis. This review will provide prospective fundamental guidance for future sulfur host design and beyond.

Potential application of Titanium carbide MXene in wearable devices is limited by the formation of voids during assembly. Here, the authors demonstrate a synergistic densification strategy by intercalating small flakes and interfacial bridging to obtain high-performance MXene films.

Abstract Zinc–selenium (Zn–Se) batteries have generated great research interest because they could potentially meet the requirements of a high‐capacity, high energy density storage device. Unfortunately, efforts to control the shuttle effect of polyselenides have yielded limited success. Nanostructured carbon hosts with nonpolar surfaces have insufficient ability to restrict polyselenides within the cathode. Herein, first‐principles calculations are used to successfully study the merits of heteroatom‐doped graphene as an efficient sorbent with an excellent ability to inhibit the shuttle effect of polyselenides. The calculation results show that using B as a dopant could distinctly enhance interaction between hosts and polyselenides, which occur significant charge transfer with polyselenides and reduce the diffusion energy barrier of Zn ions. Then, we synthesized carbon/Se and boron‐doped carbon material/Se composite cathodes proving that B‐doped carbon could restrict the shuttle effect of polyselenides, which increases the electrochemical performance of Zn–Se batteries. Therefore, the theoretical study identifies a delightful restricted material that could potentially restrict the shuttle effect in Zn–Se batteries and provides a foundation and strategy for the fabrication of long‐life, high‐power‐density Zn–Se batteries.

Abstract Constructing a conductive carbon‐based artificial interphase layer (AIL) to inhibit dendritic formation and side reaction plays a pivotal role in achieving longevous Zn anodes. Distinct from the previously reported carbonaceous overlayers with singular dopants and thick foreign coatings, a new type of N/O co‐doped carbon skin with ultrathin feature (i.e., 20 nm thickness) is developed via the direct chemical vapor deposition growth over Zn foil. Throughout fine‐tuning the growth conditions, mosaic nanocrystalline graphene can be obtained, which is proven crucial to enable the orientational deposition along Zn (002), thereby inducing a planar Zn texture. Moreover, the abundant heteroatoms help reduce the solvation energy and accelerate the reaction kinetics. As a result, dendrite growth, hydrogen evolution, and side reactions are concurrently mitigated. Symmetric cell harvests durable electrochemical cycling of 3040 h at 1.0 mA cm−2/1.0 mAh cm−2 and 136 h at 30.0 mA cm−2/30.0 mAh cm−2. Assembled full battery further realizes elongated lifespans under stringent conditions of fast charging, bending operation, and low N/P ratio. This strategy opens up a new avenue for the in situ construction of conductive AIL toward pragmatic Zn anode.

Improving the energy density of lithium-sulfur batteries is necessary for their practical application. Here, the authors report free-standing and low-tortuosity carbon frameworks as host for sulfur and lithium, enabling scalable thickness independent electrochemical performance.

Abstract The solid‐electrolyte interphase (SEI) generated between the electrode and the electrolyte strongly influences the performance of batteries. As the most attractive next‐generation energy storage system with ultrahigh energy density, the development of lithium metal batteries (LMBs) has been greatly plagued by the uncontrollable lithium (Li) dendrite and serious electrolyte decomposition resulting from the self‐derived unstable SEI with poor properties. In this perspective, the recent progress of regulating the nature and composition of the SEI to stabilize the Li metal in LMBs is summarized, followed by a discussion of the formation mechanism and the property of the SEI. The strategies for constructing a stable SEI are summarized, for example, design of a compatible electrolyte with the anode, adding self‐sacrificing additives or solvation control additives, and the regulation of nonfaradaic electric adsorption and desorption progress. Finally, the guideline for the rational design of the SEI is proposed.

Summary: Despite their widespread study, lithium metal anodes still face the bottleneck problem of low average Coulombic efficiency. Herein, we adopt an electroless plating method and introduce additive (vanillin) to develop nanoscale silver hosts. The uniform nanoscale silver layer is conducive to seamless Li/Ag alloying process, thereby enabling flat lithium deposition. Since the Li/Ag alloying process occurs after the formation of solid electrolyte interphase (SEI), the seamless alloying process stabilizes the SEI, which improves the reversibility of the lithium metal anode. On this basis, a 3D-printed copper host-coated dense nanoscale silver layer is constructed, which reduces the effective current density and hence lowers the polarization of lithium deposition or stripping. Moreover, the 3D structure induces the epitaxial growth of lithium and thus alleviates the volume change of lithium metal. As a result, an average Coulombic efficiency of 99.61% is achieved in the Li/3D Ag half-cell.

Abstract Titanium dioxide (TiO2) has gained burgeoning attention for potassium-ion storage because of its large theoretical capacity, wide availability, and environmental benignity. Nevertheless, the inherently poor conductivity gives rise to its sluggish reaction kinetics and inferior rate capability. Here, we report the direct graphene growth over TiO2 nanotubes by virtue of chemical vapor deposition. Such conformal graphene coatings effectively enhance the conductive environment and well accommodate the volume change of TiO2 upon potassiation/depotassiation. When paired with an activated carbon cathode, the graphene-armored TiO2 nanotubes allow the potassium-ion hybrid capacitor full cells to harvest an energy/power density of 81.2 Wh kg−1/3746.6 W kg−1. We further employ in situ transmission electron microscopy and operando X-ray diffraction to probe the potassium-ion storage behavior. This work offers a viable and versatile solution to the anode design and in situ probing of potassium storage technologies that is readily promising for practical applications.

Abstract Despite the significant progress in the fabrication of advanced electrode materials, complex control strategies and tedious processing are often involved for most targeted materials to tailor their compositions, morphologies, and chemistries. Inspired by the unique geometric structures of natural biomacromolecules together with their high affinities for metal species, we propose the use of skin collagen fibers for the template crafting of a novel multicore–shell Fe2N–carbon framework anode configuration, composed of hierarchical N-doped carbon nanofiber bundles firmly embedded with Fe2N nanoparticles (Fe2N@N-CFBs). In the resultant heterostructure, the Fe2N nanoparticles firmly confined inside the carbon shells are spatially isolated but electronically well connected by the long-range carbon nanofiber framework. This not only provides direct and continuous conductive pathways to facilitate electron/ion transport, but also helps cushion the volume expansion of the encapsulated Fe2N to preserve the electrode microstructure. Considering its unique structural characteristics, Fe2N@N-CFBs as an advanced anode material exhibits remarkable electrochemical performances for lithium- and potassium-ion batteries. Moreover, this bio-derived structural strategy can pave the way for novel low-cost and high-efficiency syntheses of metal-nitride/carbon nanofiber heterostructures for potential applications in energy-related fields and beyond.

Atomic-level control over size, shape and surface composition of nanoparticles is vital for developing materials with integrated multiple functionalities. Here, the authors probe the different roles of oleate ions and oleic acid molecules and their effects on growth mechanisms for sub-50 nm nanoparticles.

Gallium-based liquid metals show excellent thermal and electrical conductivities with low viscosity and non-toxicity. Their melting points are either lower than or close to room temperature, which endows them with additional advantages in comparison to the solid metals; for example, they are flexible, stretchable and reformable at room temperature. Recently, great improvements have been achieved in developing multifunctional devices by using Ga-based liquid metals, including actuators, flexible circuits, bio-devices and self-healing superconductors. Here, we review recent research progress on Gallium-based liquid metals, especially on the applications aspects. These applications are mainly based on the unique properties of liquid metals, including low melting point, flexible and stretchable mechanical properties, excellent electrical and thermal conductivities and biocompatibility.

Point defect pinning centers are the key factors responsible for the flux pinning and critical current density in type II superconductors. The introduction of the point defects and increasing their density without any changes to the superconducting transition temperature Tc, irreversibility field Hirr, and upper critical field Hc2, would be ideal to gain insight into the intrinsic point-defect-induced pinning mechanism. In this work, we present our investigations on the critical current density Jc, Hc2, Hirr, the activation energy U0, and the flux pinning mechanism in Fe1-xCoxSe0.5Te0.5 (x = 0, 0.03 and 0.05) single crystals. Remarkably, we observe that the Jc and U0 are significantly enhanced by up to 12 times and 4 times for the 3at.% Co-doped sample, whereas, there is little change in Tc, Hirr, and Hc2. Furthermore, charge-carrier mean free path fluctuation, δl pinning, is responsible for the pinning mechanism in Fe1-xCoxSe0.5Te0.5.

Abstract Lithium‐ion batteries (LIBs) with higher energy density are very necessary to meet the increasing demand for devices with better performance. With the commercial success of lithiated graphite, other graphite intercalation compounds (GICs) have also been intensively reported, not only for LIBs, but also for other metal (Na, K, Al) ion batteries. In this Progress Report, we briefly review the application of GICs as anodes and cathodes in metal (Li, Na, K, Al) ion batteries. After a brief introduction on the development history of GICs, the electrochemistry of cationic GICs and anionic GICs is summarized. We further briefly summarize the use of cationic GICs and anionic GICs in alkali ion batteries and the use of anionic GICs in aluminium‐ion batteries. Finally, we reach some conclusions on the drawbacks, major progress, emerging challenges, and some perspectives on the development of GICs for metal (Li, Na, K, Al) ion batteries. Further development of GICs for metal (Li, Na, K, Al) ion batteries is not only a strong supplement to the commercialized success of lithiated‐graphite for LIBs, but also an effective strategy to develop diverse high‐energy batteries for stationary energy storage in the future.

Aging can significantly modify the dielectric, piezoelectric, and ferroelectric performance of ferroelectrics. However, little attention has been paid to the aging effect during ferroelectric-ferroelectric phase transitions that is essentially correlated with real applications. In this letter, the authors report the aging effect evolution between two ferroelectric phases in an acceptor-doped piezoceramics. The results show that aging-induced double hysteresis loops were exhibited in different ferroelectric phases, but disappeared during ferroelectric-ferroelectric phase transitions, suggesting the mechanism that the intrinsic restoring force for the reversible switching of domains caused by the alignment of defect dipoles was weakened due to ferroelectric dipole reorientation.

Sodium-ion batteries (SIBs) as one of the promising alternatives to lithium-ion batteries have achieved remarkable progress in the past. However, the all-climate performance is still very challenging for SIBs. Herein, 15-Crown-5 (15-C-5) is screened as an electrolyte additive from a number of ether molecules theoretically. The good sodiophilicity, high molecule rigidity, and bulky size enable it to reshape the solvation sheath and promote the anion engagement in the solvated structures by molecule crowding. This change also enhances Na-ion transfer, inhibits side reactions, and leads to a thin and robust solid-electrolyte interphase. Furthermore, the electrochemical stability and operating temperature windows of the electrolyte are extended. These profits improve the electrochemical performance of SIBs in all climates, much better than the case without 15-C-5. This improvement is also adopted to μ-Sn, μ-Bi, hard carbon, and MoS2. This work opens a door to prioritize the potential molecules in theory for advanced electrolytes. [ABSTRACT FROM AUTHOR]