Functionalization has emerged as a pivotal endeavor to tailor the surface properties of photocatalysts. We propose a facile amine functionalization strategy to establish a Cu−In−Zn−S (CIZS)/NiS_x hybrid with covalent bonds using individual ethylenediamine (EDA) molecules. Our approach witnesses a remarkable photocatalytic hydrogen evolution (PHE) competence of 65.93 mmol g⁻¹ h⁻¹ driven by visible light, the highest value yielded by CIZS to date. X-ray absorption spectra of CIZS and density functional theory (DFT) calculations confirm the crucial amine N→Cu coordination after amine functionalization. The new emerging coordination via lone-pair electron donation profitably accesses the regulation of the coordination environment, electronic structures, and carrier behavior. Moreover, individual EDA molecule with two-terminal −NH₂ group serves as a molecular bridge to hybrid CIZS and NiS_x cocatalyst via N→Cu and N→Ni coordination, favorably promoting efficient charge transport. This study provides advances in practical functionalizing photocatalysts.

The development of human industry inevitably leads to excessive carbon dioxide (CO₂) emissions. It can cause critical ecological consequences, primarily global warming and ocean acidification. In this regard, close attention is paid to the carbon capture, utilization, and storage concept. The key component of this concept is the catalytic conversion of CO₂ into valuable chemical compounds and fuels. Light olefins are one of the most industrially important chemicals, and their sustainable production via CO₂ hydrogenation could be a prospective way to reach carbon neutrality. Fe-based materials are widely recognized as effective thermocatalysts and photothermal catalysts for that process thanks to their low cost, high activity, and good stability. This review critically examines the most recent progress in the development and optimization of Fe-based catalysts for CO₂ hydrogenation into light olefins. Particular attention is paid to understanding the roles of catalyst composition, structural properties, and promoters in enhancing catalytic activity, selectivity, and stability.

The recovery and utilization of ubiquitous low-grade heat are crucial for mitigating the fossil energy crisis. However, uncontrolled spontaneous heat dissipation limits its practical application. Inspired by skeletal muscle thermogenesis, we develop a compressible wood phase change gel with mechano-controlled heat release by infiltrating xylitol gel into wood aerogel. The xylitol gel can store recovered low-grade heat for at least 1 month by leveraging its inherent energy barrier. The hierarchically aligned lamellar structure of wood aerogel facilitates mechanical adaptation, hydrogen bond formation, and energy dissipation between the wood aerogel and the xylitol gel, increasing the compressive strength and toughness of wood phase change gel fivefold compared to xylitol gel. This enhancement effect enables repetitive contact-separation motions between the wood phase change gel and the substrate during radial compression, overcoming the energy barrier and releasing approximately 178.6 J g⁻¹ of heat. As a proof-of-concept, the wood phase change gel serves as the hot side in a thermoelectric generator, providing about 2.13 W m⁻² of clean electricity by the controlled utilization of recovered solar heat. This study presents a sustainable method to achieve off-grid electricity generation through the controlled utilization of recovered low-grade heat.

Hard carbon is the most commercially viable anode material for sodium-ion batteries (SIBs), and yet, its practical implementation remains constrained by insufficient low-voltage plateau capacity, a critical parameter governing storage capacity. This study introduces a targeted component removal and chemical etching strategy to precisely tailor the porous structure of hard carbon and thus remarkably enhance the plateau capacity. In this strategy, alkaline-dissolved components are removed to form a closed-pore core with tunable size. Subsequently, the in situ occupied alkaline engineers the pore structure through chemical etching. The optimized hard carbon material not only has short-range disordered graphite domains to facilitate Na⁺ ions' intercalation and deintercalation but also has abundant micropores and closed-pore structures with appropriate pore sizes and an ultrathin carbon layer (1−3 layers) to significantly increase the sodium storage sites. The resulting hard carbon delivers a high reversible specific capacity of 389.6 mAh g⁻¹ with a low-voltage plateau capacity as high as up to 261.5 mAh g⁻¹ and an initial Coulombic efficiency of 90.7%. Crucially, this cost-effective methodology shows broad precursor adaptability across lignocellulosic biomass, establishing a universal paradigm for designing high-performance carbonaceous anodes for SIBs.

The efficient storage and application of sustainable solar energy has drawn significant attention from both academic and industrial points of view. However, most developed catalytic materials still suffer from insufficient mass diffusion and unsatisfactory durability due to the lack of interconnected and regulatable porosity. Developing catalytic architectures with engineered active sites and prominent stability through rational synthesis strategies has become one of the core projects in solar-driven applications. The unique properties of mesoporous silicas render them among the most valuable functional materials for industrial applications, such as high specific surface area, regulatable porosity, adjustable surface properties, tunable particle sizes, and great thermal and mechanical stability. Mesoporous silicas serve as structural templates or catalytic supports to enhance light harvesting via the scattering effect and provide large surface areas for active site generation. These advantages have been widely utilized in solar applications, including hydrogen production, CO₂ conversion, photovoltaics, biomass utilization, and pollutant degradation. To achieve the specific functionalities and desired activity, various types of mesoporous silicas from different synthesis methods have been customized and synthesized. Moreover, morphology regulation and component modification strategies have also been performed to endow mesoporous silica-based materials with unprecedented efficiency for solar energy storage and utilization. Nevertheless, reviews about synthesis, morphology regulation, and component modification strategies for mesoporous silica-based catalyst design in solar-driven applications are still limited. Herein, the latest progress concerning mesoporous silica-based catalysis in solar-driven applications is comprehensively reviewed. Synthesis principles, formation mechanisms, and rational functionalities of mesoporous silica are systematically summarized. Some typical catalysts with impressive activities in different solar-driven applications are highlighted. Furthermore, challenges and future potential opportunities in this study field are also discussed and proposed. This present review guides the design of mesoporous silica catalysts for efficient solar energy management for solar energy storage and conversion applications.

The high chloride (Cl) concentration in seawater presents a critical challenge for hydrogen production via seawater electrolysis by deactivating catalysts through active site passivation, highlighting the need for catalyst innovation. Herein, in situ boron-doped Co₂P/CoP (B-Co_xP) ultrathin nanosheet arrays are prepared as high-performance bifunctional electrocatalysts for seawater decomposition. Density functional theory (DFT) simulations, comprehensive characterizations, and in-situ analyses reveal that boron doping enhances electron density around Co centers, induces lattice distortions, and significantly elevates catalytic activity and durability. Moreover, boron doping reduces *Cl retention time at active sites—defined as the DFT-derived residence time of adsorbed Cl intermediates based on their adsorption energies—effectively mitigating Cl-induced poisoning. In a three-electrode system, B-Co_xP achieves exceptional bifunctional performance with overpotentials of 11 mV for hydrogen evolution reaction and 196 mV for oxygen evolution reaction to deliver 10 and 50 mA·cm^–2, respectively—a result that showcases its superior bifunctional properties surpassing noble metal-based counterparts. In an alkaline electrolyzer, it delivers 1.56 A·cm^–2 at 2.87 V for seawater electrolysis with outstanding stability over 500 h, preserving active site integrity via boron's robust protective role. This study defines a paradigm for designing advanced seawater electrolysis catalysts through a strategic in-situ doping approach.

Copper complexes inspired by O₂-activating enzymes have been widely investigated as molecular water oxidation catalysts, capable of facile and reversible O─O bond formation and cleavage under mild conditions. In this study, two copper phenanthroline complexes, namely, Cu(phen) and Cu(dophen), exhibit high turnover frequencies (TOFs) of 74 ± 13 and (5.66 ± 0.29) × 10³ s⁻¹ for water oxidation, respectively. Moreover, amino acid-functionalized carbon dots (CDs) were used to support the adhesion of the [Cu] complexes onto the electrode, significantly enhancing the TOFs of (2.80 ± 0.12) × 10³ and (4.11 ± 0.24) × 10⁴ s⁻¹, respectively, exceeding the activity of photosystem II in nature. Remarkably, the amino acid-functionalized CDs provide a secondary sphere that mimics the catalytic microenvironment of the copper centre, which promotes proton-coupled electron transfer and O─O bond formation. Finally, the photovoltaic-electrolysis (PVE) system was established using CDs-supported Cu catalysts and commercial silicon solar panels, achieving a high solar-to-hydrogen efficiency of 11.59% under the illumination of AM 1.5 G. This represents the most efficient solar-driven water splitting system based on copper-based catalysts to date, introducing the biomimetic secondary sphere to a “proton-rocking” process for water oxidation catalysis and application of the PVE system.

Developing low-cost and efficient catalysts for sustainable hydrogen (H₂) production to the reliance on precious metal is an important trend in the future development of catalysts. Herein, a simple in-situ one-step hydrothermal strategy is employed to modify the outer layer of Ni₃S₂ crystals with amorphous MoS₂ to construct core-shell heterostructures and heterogeneous interfaces, which promotes the chemisorption of intermediates, including hydrogen and oxygen, and realizes the coupling enhancement of hydrogen-evolution reaction (HER) and oxygen-evolution reaction (OER) in alkaline water electrolysis process. In 1.0 M KOH electrolyte, the overpotentials of the electrodes are 78 mV (HER) and 245 mV (OER) at a current density of 10 mA cm⁻², respectively. At the same time, the electrode has excellent stability for more than 100 h at a current density of 100 mA cm⁻², due to the amorphous structure. In addition, when used as an anode and cathode to form an electrolyzer, a cell voltage of only 1.5 V is required to produce a current density of 10 mA cm⁻². This study demonstrates that the constructed amorphous heterostructured interface synergistically promotes the dissociation of water and the adsorption of intermediates, providing a deep insight on how to accelerate the development of efficient catalysts.

Electrides, in which anionic electrons are trapped in structural cavities, have garnered significant attention for exceptional functionalities based on their low work function. In low-dimensional electrides, a strong quantum confinement of anionic electrons leads to many interesting phenomena, but a severe chemical instability due to their open structures is one of the major disadvantages for practical applications. Here we report that one-dimensional (1D) dititanium sulfide electride exhibits an extraordinary stability originating from the surface self-passivation and consequent durability in bifunctional electrocatalytic activity. Theoretical calculations identify the uniqueness of the 1D [Ti₂S]²⁺·2e⁻ electride, where multiple cavities form two distinct channel structures of anionic electrons. Combined surface structure analysis and in-situ work function measurement indicate that the natural formation of amorphous titanium oxide surface layer in air is responsible for the remarkable inertness in water and pH-varied solutions. This makes the [Ti₂S]²⁺·2e⁻ electride an ideal support for a heterogenous metal-electride hybrid catalyst, demonstrating the enhanced efficiency and superior durability in both the hydrogen evolution and oxygen reduction reactions compared to commercial Pt/C catalysts. This study will stimulate further exploratory research for developing a chemically stable electride in reactive conditions, evoking a strategy for a practical electrocatalyst for industrial energy conversions.

Full-manganese (Mn) Li-rich materials have gained attention owing to the limited availability of cobalt- or nickel-based cathodes commonly used in batteries, which greatly restricts their potential for large-scale application. However, their practical implementation is hindered by the rapid voltage/capacity decay during cycling and the long-standing problem of redox kinetics due to their poor ionic conductivity based on the ordered honeycomb structure. In this study, the kinetic and thermodynamic properties of intralayer disordered and ordered Li-rich full-Mn-based cathode materials were compared, demonstrating that the disordered R\overline{3} m Li_0.6[Li_0.2Mn_0.8]O₂ (O-LMO). Meanwhile, the D-LMO keeps superior capacity retention of up to 99% after 50 cycles under 25 mA g⁻¹. In comparsion, the capacity retention of the O-LMO drops to just 70%, and its average discharge voltage is 0.2 V lower than that of the D-LMO. Herein, we conducted systematic density functional theory (DFT) simulations, focusing on the electronic structure modulation governing the voltage platform between the ordered and disordered phases. The ab initio molecular dynamics (AIMD) results indicated that the energy of the intralayer disordered structure fluctuates around the equilibrium position without any abrupt drops, demonstrating excellent stability. This study enhances the understanding of intralayer disordered full-Mn Li-rich material and provides insights into the design of low-cost, high-performance cathode materials for Li-ion batteries.

Polarization-dependent loss is important to the highly electromagnetic wave absorption (EWA) performance. Recently, metal–N_x moieties have been discovered to trigger polarization loss, but the physical origin and other possible related loss mechanisms still need to be deeply explored. In this article, we reveal that the FeN₄ moiety from iron phthalocyanine (FePc) can coordinate with Ti₃C₂T_x through Ti–OH groups, inducing dipole polarization and synchronous magnetic modulation in Fe/TiO₂/Ti₃C₂T_x composites. Interestingly, using the enhanced electric dipole moment and increased number of unpaired electrons in Fe atoms, the dipole polarization loss and possible magnetic response can be rapidly confirmed and evaluated. As a result, the minimum reflection loss (RL_min) of Fe/TiO₂/Ti₃C₂T_x composites reaches −67.12 dB at 6.72 GHz with a thickness of 3.32 mm. This study elaborates the EWA mechanism based on the atomic scale, and provides a new idea to design efficient EWA materials.

Copper–carbon (Cu–C) composites have achieved great success in various fields owing to the greatly improved electrical properties compared to pure Cu, for example, a two-order-of-magnitude increase in current-carrying capacity (ampacity). However, the frequent fuse failure caused by the poor thermal transport at the Cu–C heterointerface is still the main factor affecting the ampacity. In this study, we unconventionally leverage atomic distortion at Cu grain boundaries to alter the local atomic environments, thereby placing a premium on noticeable enhancement of phonon coupling at the Cu–C heterointerface. Without introducing any additional materials, interfacial thermal transport can be regulated solely through rational microstructural design. This new strategy effectively improves the interfacial thermal conductance by three-fold, reaching the state-of-the-art level in van der Waals (vdW) interface regulation. It can be an innovative strategy for interfacial thermal management by turning the detrimental grain boundaries into a beneficial thermal transport accelerator.