Guihua Yu

ABSTRACT Hygroscopic hydrogels have emerged as promising candidates for sorbent‐based atmospheric water harvesting (AWH) technologies. However, most hydrogels are composed of petroleum‐derived synthetic monomers, raising concerns regarding the sustainability of AWH in water management. Although natural polymers and their derivatives are considered alternative resources, they often require complex processing with multiple chemicals to achieve advanced properties, thereby reducing their cost‐effectiveness and environmental friendliness. In this context, this study presents a simple and direct strategy for synthesizing hygroscopic hydrogels from gelatin. Through pH adjustment, gelatin's protonated amine and deprotonated carboxyl groups are activated, resulting in polyzwitterionic‐like properties and tailorable salting‐in effect. Furthermore, the intermolecular bonding network of gelatin can be further disrupted by specific ions via Hofmeister effects. Consequently, the charge‐engineered gelatin (CEG) sorbent achieves a water uptake of 0.92 g g −1 at 30% relative humidity. In practical applications, when incorporated with a photothermal agent, this sorbent can produce 2.7 L m −2 day −1 of desorption under sunlight. The CEG‐based sorbent provides an accessible, cost‐effective AWH material while maintaining sufficient efficiency to meet daily water requirements.

Sorption-based atmospheric water harvesting (AWH) offers a decentralized, sustainable solution to global freshwater scarcity, enabling clean water in diverse environments. However, translating ideal sorption properties of small-scale materials into practical, large-scale systems faces critical kinetic challenges. Here, we conceptualize a hierarchical textile fiber for wearable AWH, addressing the scaling limitations of traditional sorbents. These fibers feature an open-pore surface topology and internal hierarchical pore structures, which accelerate surface vapor liquefaction and subsequent water transport, demonstrating exceptional water uptake and rapid sorption kinetics across varying relative humidity (RH). When woven into textiles, the fibers maintain efficient vapor diffusion through their macroporous, breathable architecture, achieving a 3- to 10-fold improvement over traditional sorbents at scale. We engineered a wearable prototype combining the AWH textile with a portable collector, achieving 3.76 to 7.45 liters water per kilogram sorbent per day and collecting 410 to 894 milliliters across 20 to 80% RH. By overcoming kinetic limitations, our study advances AWH toward scalability and wearability with implications for global water sustainability.

Atmospheric water harvesting (AWH) offers a promising solution to the escalating global water crises. Among its variants, sorption-based AWH (SAWH) is particularly notable for its adaptability across a range of climates. In this Review, we delve into the complexities of sorbent materials, discussing foundational sorption dynamics, advances in material design, and the strategies for scale-up processing. The analysis extends to system engineering, particularly the optimization of thermal and mass-transfer processes essential for effective operation across different scenarios. By synthesizing insights from materials, systems, and climate, we tackle the challenges of energy management, operational strategies, and multifunctional applications. We outline a strategic roadmap for the practical implementation of SAWH technologies, underscoring their potential to significantly enhance sustainable water solutions globally.

This study integrates computational fluid dynamics (CFD) simulations with machine learning (ML) models to develop a framework for predicting drug release from hydroxypropyl methylcellulose (HPMC) matrices. Transient, three-dimensional CFD models were constructed to solve the conservation equations for fluid flow and mass transfer, explicitly simulating the swelling front propagation, polymer dissolution, and diffusive drug release from a cylindrical HPMC carrier into a dissolution medium. The key results from parametric CFD studies quantified the nonlinear relationship between initial drug loading and the resultant concentration gradients and release rates over time, providing a high-resolution dataset on the underlying transport phenomena. These CFD simulations were validated against experimental release data, achieving excellent agreement (mean absolute error of 1.54% and R-squared of 0.9997). The CFD-generated data, combined with experimental measurements from the literature for eight model drugs (ribavirin, ranitidine hydrochloride, isoniazid, diltiazem hydrochloride, theophylline, tinidazole, sulfamethoxazole, and propylthiouracil), were used to train the machine learning techniques. A systematic topology search identified an optimized least-squares support vector regression (LS-SVR) as the most accurate predictor. This LS-SVR model, configured with the Gaussian kernel function, successfully predicts the overall dataset with an R-squared of 0.99850, an average absolute relative deviation of 1.27%, and a root mean squared error of 0.833. This hybrid CFD-ML approach provides a powerful tool for the rational design of HPMC-based drug formulations with targeted release profiles.

Interfacial solar vapor generation (SVG) has emerged as a promising strategy for water purification and desalination. Among SVG technologies, hydrogel-based evaporators stand out for their high energy efficiency and effective evaporation, but their performance often collapses under high irradiance due to insufficient water transport. Here we develop an ultralow-density rigid-network (ULR) hydrogel engineered for ultrafast water transport and evaporation. The ULR network maximizes water content and establishes steep osmotic-pressure gradients for rapid water supply, while the rigid, anti-shrinkage framework preserves hierarchical pores, sustaining capillary-driven flow and maintaining continuous vapor production under extreme irradiance. ULR evaporators surpass traditional hydrogels’ theoretical maximum water transport rate, achieving an evaporation rate of 25.57 kg m⁻² h⁻¹ at 10 suns for 100 h. In practical trials, a low-cost module produced 138 L m⁻² day⁻¹, yielding 12.42 L day⁻¹ of potable water. This design advances hydrogel-based SVG toward robust, affordable solutions for real-world water scarcity. Researchers developed ultralow-density rigid-network hydrogels for stable solar desalination under intense sunlight. They reach an evaporation rate of 25.57 kg m⁻2 h⁻1 at 10 suns and deliver water production of 138 L m⁻2 day⁻1 in low-cost modules.

The deployment of renewable energy necessitates reliable grid-scale storage technologies. Aqueous metal battery systems are one of the promising candidates due to high safety, low cost, and high theoretical capacity of metal anodes, yet their long-term stability is hindered by dendritic growth and parasitic water-induced side reactions. In particular, in the case of aqueous zinc (Zn) batteries, high water reactivity at the metal anode results in hydrogen evolution and corrosion in conventional ZnSO 4 aqueous electrolytes. However, restrained water activity often leads to slow charge transport kinetics of solvated cations, limiting the high-rate operation capability of aqueous batteries. Here, we report a gradient composite hydrogel interlayer incorporating vermiculite (VMT) nanosheets within a polyacrylamide polymer matrix to synergistically regulate interfacial water dynamics and stabilize Zn anodes. Abundant hydroxyl groups and negatively charged silicate layers in VMT nanosheets strongly interact with adjacent water molecules, converting free water into bound water to suppress its activity. Charge transport behaviors of Zn ions in the hydrogel interlayer are further improved by rationally tuning the water activity along the depth of the interlayer, resulting in high ion diffusion kinetics close to the bulk electrolyte. Therefore, such a design enables Zn||Zn symmetric cells to stably cycle for over 2,000 h at 5 mA cm −2 and 5 mAh cm −2 , and sustain high current densities up to 40 mA cm −2 . This work brings critical scientific understanding on interfacial water dynamics and highlights its importance for durable metal anode during operation, advancing aqueous batteries toward practical grid-scale energy storage.

Rechargeable batteries using electrodes based on intercalation chemistry exhibit notable cyclability, yet their performance still suffers from chemomechanical degradation. In this study, by combining a suite of operando microscopy methods, we explored electrode strain evolution and observed intricate particle cluster rearrangement under electrochemical stimuli. We show that early-stage strain accumulation in intercalation cathodes occurs during the period of interparticle charge transfer and redox reactions stemming from asynchronous coupling and decoupling between chemical (de)intercalation and physical grain motion. This interplay drives heterogeneous redox activity, localized charge equilibration, and multiscale strain cascades that propagate through an asynchronous network of chemical-mechanical interactions. Together, these findings reveal how collective particle dynamics and hierarchical strain transmission dictate electrode deformation and degradation in intercalation cathodes.

Magnesium metal batteries are considered promising candidates for next-generation energy storage systems due to the high volumetric capacity, intrinsic safety and natural abundance of magnesium. Yet, the fundamental mechanisms that govern the magnesium deposition and the formation of surface interphases remain poorly understood, largely due to the complexity of battery chemistry and the lack of reliable techniques to probe these processes at the atomic scale. Here we show that, by using cryogenic transmission electron microscopy, different magnesium deposition morphologies (e.g., whisker-shaped or seaweed-shaped) in conventional single-salt electrolytes converge to an intrinsic hexagonal platelet shape once surface passivation is decoupled from magnesium plating. This characteristic shape persists across different electrolyte chemistries, suggesting that suppressing surface passivation eliminates the influence of electrolyte composition on magnesium deposition morphology. These findings reveal the intrinsic nature of magnesium electrodeposition and establish a mechanistic link between interfacial chemistry and morphological evolution. Our work highlights a fundamental principle for controlling magnesium deposition behavior, paving the way for the rational design of stable, high-performance magnesium-based batteries. Magnesium metal batteries hold great promise for next-generation energy storage but struggle with limited understanding of their deposition mechanisms. Here, authors employ cryogenic electron microscopy to uncover how interfacial chemistry governs magnesium deposition across diverse electrolytes.

characterization techniques are highlighted, through which dynamic insights into catalyst evolution and intermediate behaviour have been obtained. Finally, opportunities are outlined for future development, where rational catalyst design, integrated system construction, and data-driven optimization are expected to further advance cascade electrocatalysis for sustainable chemical transformations.

Electrochemical CO 2 reduction to single-carbon products is central to sustainable fuels and chemicals, but under industrially relevant conditions elevated temperature fundamentally alters reaction behavior and the mechanistic basis for steering hydrogenation of carbon-based intermediates toward selective C 1 formation remains elusive. By integrating artificial intelligence-guided literature mining with theoretical modeling, single-atom alloy catalysts combining thermodynamic advantage with temperature-dependent dynamic surface stability were identified. We report that the coverage and lifetime of surface-active hydrogen (*H) serve as intrinsic, temperature-dependent descriptors for catalyst design, enabling tunable C 1 activity and selectivity under thermally enhanced electrocatalysis. Au 1 Cu single-atom alloys are shown to direct CO 2 to either CO or CH 4 via thermally stabilized hydrogenation dynamics; in situ surface-interrogation scanning electrochemical microscopy quantitatively resolves *H coverage and lifetime and links their balance to suppression of hydrogen evolution and promotion of deep hydrogenation to methane. Selectivity was modulated by Au content, delivering about 60% faradaic efficiency for CH 4 at 353 K, whereas higher loadings favored approximately 85–90% CO. Under device-relevant operation and high renewable electricity share, net carbon emissions were reduced relative to conventional electrocatalysis. These findings highlight a quantitative, temperature-explicit mechanistic framework based on *H coverage and lifetime, providing general principles for C 1 -selective CO 2 electroreduction and guiding catalyst design beyond room-temperature conditions.

Given the growing emphasis on energy efficiency, environmental sustainability, and agricultural demand, there’s a pressing need for decentralized and scalable ammonia production. Converting nitrate ions electrochemically, which are commonly found in industrial wastewater and polluted groundwater, into ammonia offers a viable approach for both wastewater treatment and ammonia production yet limited by low producibility and scalability. High-entropy materials (HEMs) is emerging as a promising class of catalytic materials with unique physicochemical properties for complex electrochemical reactions such as ammonia electrosynthesis from nitrate. However, the high compositional complexity of HEMs often frustrates the effort for manipulating their morphology and surface structures without compromising their versatility and scalability. Here we report a scalable solution-phase synthesis of high-entropy single-atom nanocages (HESA NCs) in which Fe and other five metals-Co, Cu, Zn, Cd, and In-are isolated via cyano-bridges and coordinated with C and N, respectively. Incorporating and isolating the five metals into the matrix of Fe resulted in Fe-C 5 active sites with a minimized symmetry of lattice as well as facilitated water dissociation and thus hydrogenation process. As a result, the Fe-HESA NCs exhibited a high selectivity toward NH3 from the electrocatalytic reduction of nitrate with a Faradaic efficiency of 93.4% while maintaining a high yield rate of 81.4 mg h −1 mg −1 .

Aluminum–sulfur (Al–S) batteries are regarded as promising electrochemical energy storage systems due to their high energy density, cost-effectiveness, and environmental compatibility. However, their practical application is hindered by sluggish sulfur conversion kinetics. Although certain achievements have been made, conventional strategies for modulating the spin state of electrocatalysts, such as heteroatom doping or lattice strain engineering, exhibit inherent limitations in optimizing electron orbital interactions. Herein, we report a novel MoS 2 electrocatalyst with spin orientation manipulation achieved through the chiral-induced spin selectivity (CISS) effect. This approach couples chiral molecules with layered MoS 2 to regulate the spin polarization of molybdenum atoms, thereby enhancing the sulfur redox kinetics without relying on chemical modification. Electrochemical analyses demonstrated that the cathode with chiral MoS 2 delivers a reversible specific capacity of ∼700 mAh g –1 at 2 A g –1 over 3000 cycles, accompanied by improved sulfur utilization efficiency. This work not only provides a paradigm for designing high-performance electrocatalysts in sulfur-based batteries but also highlights the critical role of spin effects in electrocatalytic systems, offering new perspectives for the innovation of electrocatalyst materials in batteries.

The increasing demand for sustainable materials has driven interest in harnessing renewable resources to develop advanced biomaterials. Cellulose nanofibers, derived from abundant natural reserves, offer excellent mechanical strength and thermal stability but lack inherent biofunctionality. This study presents a method that is green, cost-effective, and scalable to synthesize amino-cellulose nanofibers (A-CNFs) by grafting carboxyl groups and thereon amino groups onto cellulose, followed by ultrasonic nanofibrillation, resulting in ultrafine, lengthy A-CNF with enhanced mechanical properties, biocompatibility, and antibacterial activity. Comparative analyses demonstrate that A-CNF scaffolds exhibit favorable biostability, pore connectivity, and mechanical integrity in tissue engineering applications. Biological assessments further indicate improved cell viability and reduced hemolysis, underscoring A-CNF's potential as robust, biocompatible, and sustainable material platforms for biomedical use.

Conspectus Facing the growing stress on freshwater supplies, harvesting water from the atmosphere via sorbents has garnered significant attention due to its broad applicability, regardless of geographic and hydraulic restrictions. In advancing the sustainable development, two critical aspects are the use of biomass-derived sorbents and solar energy. Biopolymers offer viable alternatives to petroleum-derived synthetic polymers, presenting opportunities for developing environmentally friendly AWH systems. Additionally, efficient capture and utilization of solar energy to drive water desorption are also critical to enhancing the sustainability of AWH. This account discusses the challenges and strategies in efficiently utilizing biomass and solar energy for sustainable AWH. We begin with the key challenges in these two domains. Transforming biomass into efficient sorbents necessitates molecular and structural engineering to achieve high water uptake capacities and rapid sorption–desorption kinetics. The inherently intermittent and relatively low power density of solar energy introduces additional energy challenges, demanding heat and mass transfer management to maximize sunlight utilization. We then highlight various strategies to mitigate these challenges and thus promote water yield in sustainable AWH systems. To endow biopolymer-based hydrogels with enhanced hygroscopicity and hydrability, extracting nanofibrils from biomass has proven effective via exposing more active sites (e.g., hydroxyl groups), significantly enhancing water uptake capacities. Chemical modifications, such as introducing zwitterionic groups, have also been demonstrated to promote polymer swelling and water capture. Structurally engineered biopolymer hydrogels further facilitate internal water diffusion, accelerating sorption and desorption. To address the energy challenges, developing thermoresponsive sorbents that release water under lower, solar-compatible temperatures is beneficial. Additionally, exploring advanced solar absorbers with high absorptivity and selective thermal emission properties can maximize solar energy capture and minimize radiative heat losses. Device-level designs that reduce radiative heat exchange and minimize view factors between sorbents and other components further contribute to efficient thermal management. Integrating heat recovery, such as reusing latent heat released from water condensation, can further improve the overall energy utilization efficiency. Efficient water transport is also essential for improving overall water yield. Employing low-dimensional sorbents like two-dimensional thin films and microgels can accelerate water diffusion within sorbents with reduced effective diffusion length. Alternatively, directional pores can be introduced in bulk sorbents to reduce tortuosity, which also benefits internal diffusion. Moreover, by introducing forced convection, the actively driven airflow can efficiently carry water vapor away from sorbent surfaces toward condenser, preventing local vapor accumulation and suppressing the humidity buildup that would otherwise inhibit further desorption. Finally we highlight future challenges and opportunities in promoting sustainable AWH.

The synergistic Cu0-Cuδ+ sites are found as the active sites for NH3 synthesis through nitrate electroreduction reaction, but still face significant challenges in stabilizing the Cuδ+ due to its self-reduction. Here we propose an Ohmic contact interface engineering strategy by loading copper nano-islands on indium hydroxide nanocubes. Attributed to the lower work function of Cu than that of In(OH)3 with n-type semiconductor nature, the electrons in Cu can transfer unimpededly to In(OH)3 at the interface of Ohmic junction, triggering and stabilizing polarized Cu0-Cuδ+ active sites. Cu@In(OH)3 sustains both high NH3 yield rate (4.28 mmol h−1 mgcat.−1) and Faradaic efficiency (97.35%) at −0.6 V vs. RHE, while maintaining stability for at least 120 h under an Ampere-level of 800 mA cm−2. Such Ohmic contact interface engineering approach allows for simultaneously constructing and stabilizing the Cu0-Cuδ+ for the electrosynthesis of ammonia, as well as other value-added chemicals relying on above active sites. An Ohmic contact interface engineering strategy was proposed by loading copper nano islands on indium hydroxide nanocubes, which could trigger and stabilize the polarized Cu0 -Cuδ+ active sites. Such catalyst enabled effective ammonia electrosynthesis with nitrate under ambient conditions

Abstract Lithium‐ion batteries, as sustainable alternatives to fossil fuels, are in great demand for powering modern society. Their energy density can further be significantly improved by using Li metal anodes; however, Li metal suffers from the critical challenges of unstable solid‐electrolyte interphase (SEI) along with uncontrollable dendritic Li growth. Here, a universal electrolyte design principle is proposed and demonstrated by using suspension electrolytes with charged additives. The solvation structure of Li ions can be regulated, as negatively charged additives show strong electrostatic interaction with Li ions, leaving them weakly solvated in the electrolyte. Moreover, negatively charged additives carrying Li ions can be locally concentrated at the surface of the Li metal, enhancing their ability to regulate solvation and improve interfacial mobility, beneficial for the formation of inorganic‐rich SEIs and compact Li deposition. Accordingly, Li||Li symmetric cell demonstrates >500 h stable cycling at 2 mA cm −2 and 2 mA h cm −2, and Li||LiFePO 4 cell shows 97% capacity retention after 400 cycles in 1C. The universality of this design is further demonstrated in various negatively charged suspension electrolyte systems. Such an electrolyte design rationale can shed light on the development of advanced electrolyte systems for realizing high‐energy‐density and long‐duration metal battery systems.

Abstract Aqueous redox flow batteries (AQRFBs) are revolutionizing energy storage by integrating sustainability with cutting‐edge innovation. Among them, Iron‐Chromium RFBs (Fe‐Cr RFBs), which utilize aqueous‐based electrolytes, effectively address critical challenges in renewable energy integration while offering unparalleled safety, low‐cost scalability and environmental compatibility. Potassium hexacyanochromate (K 3 [Cr(CN) 6 ]) has emerged as a promising negolyte material in Fe‐Cr RFBs due to its favorable electrochemical properties. However, enhancing its long‐term stability and elucidating its structural transformations remain crucial for optimized performance. Investigations into ligand exchange mechanism reveal connections to detrimental side reactions, notably hydrogen evolution reaction (HER) and hexacyanochromate instability, highlighting pathways for targeted improvement. Density functional theory (DFT) calculations illuminate the effects of ligand exchange dynamics and structural variations on redox stability, providing mechanistic insights into electrolyte behavior. By strategically incorporating sodium hydroxide with sodium cyanide as supporting electrolytes, our study demonstrates significantly improved stability of the redox couple, achieving a stable cycling performance over 250 cycles with an energy density of 13.91 Wh L −1 and energy efficiencies exceeding 76%–77%. This research provides valuable insights into the degradation pathways of hexacyanochromate‐based negolyte and emphasizes the importance of optimized electrolyte design for advancing sustainable energy storage technologies.

Abstract Aqueous redox flow batteries (AQRFBs) are revolutionizing energy storage by integrating sustainability with cutting‐edge innovation. Among them, Iron‐Chromium RFBs (Fe‐Cr RFBs), which utilize aqueous‐based electrolytes, effectively address critical challenges in renewable energy integration while offering unparalleled safety, low‐cost scalability and environmental compatibility. Potassium hexacyanochromate (K 3 [Cr(CN) 6 ]) has emerged as a promising negolyte material in Fe‐Cr RFBs due to its favorable electrochemical properties. However, enhancing its long‐term stability and elucidating its structural transformations remain crucial for optimized performance. Investigations into ligand exchange mechanism reveal connections to detrimental side reactions, notably hydrogen evolution reaction (HER) and hexacyanochromate instability, highlighting pathways for targeted improvement. Density functional theory (DFT) calculations illuminate the effects of ligand exchange dynamics and structural variations on redox stability, providing mechanistic insights into electrolyte behavior. By strategically incorporating sodium hydroxide with sodium cyanide as supporting electrolytes, our study demonstrates significantly improved stability of the redox couple, achieving a stable cycling performance over 250 cycles with an energy density of 13.91 Wh L −1 and energy efficiencies exceeding 76%–77%. This research provides valuable insights into the degradation pathways of hexacyanochromate‐based negolyte and emphasizes the importance of optimized electrolyte design for advancing sustainable energy storage technologies.

The development of sustainable artificial nitrogen recycling technologies enables ammonia extraction from ambient sources, facilitating zero-carbon Water-Energy-Food (WEF) Nexus integration. While electrochemical reduction of oxidized nitrogen offers promise for ammonia synthesis, purifying low-concentration products remains a challenge, limiting practical applications and undermining the Haber-Bosch process’s viability. Here, we introduce a photothermal-electrocatalysis interface (PTEI) based on a Janus hybrid nanoarchitecture electrode, demonstrating synergistic enhancement in ammonia yield and evaporation performance. The photothermal-electrocatalysis interface-integrated system continuously produces and purifies ~2 M pure ammonia solution at up to 13.7 mg cm−2 h−1 from plasma-ionized air and achieves 80% total nitrogen recovery with 0.36 M ammonia from simulated industrial wastewater. This approach enables efficient extraction of concentrated ammonia for direct fuel cell use, offering techno-economic benefits and significantly reducing global warming impacts via life cycle assessment. Our findings highlight the PTEI system’s innovative potential in addressing WEF Nexus challenges, paving the way for sustainable waste-to-resource/fuel transitions. The authors report a dual photothermal-electrocatalysis interface which enables efficient ammonia extraction and purification from air and wastewater, thereby advancing sustainable waste-to-fuel conversion.

Interfacial solar-driven evaporation has attracted great research interests, given its high conversion efficiency of solar energy and transformative industrial potential for desalination. However, current evaporators with porous volume remain critical challenges by inherently balancing efficient fluid transport and effective heat localization. Herein, we propose the strategy and design of lightweight, flexible and monolayered fluidic diode membrane-based evaporators, featuring regularly arrayed macropores and dense nanopores on each side. Such a delicate microstructure offers universality in establishing asymmetric channels along macroporous-to-nanoporous to enable the diode-like directional water transport as well as facilitate the heat localization on the nanopores side. Consequently, a high evaporation rate of a maximum 3.82 kg m−2 h−1 can be achieved under 1 sun illumination, exceeding most 2D and 3D evaporators. Besides, the durability and practicability of our evaporators are validated through salt resistance tests, purification experiments among various contaminants, and outdoor evaluations. Moreover, the structure engineering and water-transport optimization of fluidic diode membranes also offer potentials for hydrovoltaic applications, with over 1.6 V generated by tandem devices at the ambient environment. This work provides a concept for designing high-performance monolayered membranes applicable in environmental and energy-related realms. Solar-powered desalination is a sustainable approach to generate clean water for our society. Here, authors report lightweight, flexible, and fluidic-diode membrane-based evaporators to allow directional water transport and optimized heat localization. This Janus evaporator design enables high performance interfacial solar water evaporation, as well as hydrovoltaic applications.

The increasing demand for high-energy-density rechargeable batteries has spurred significant advancements in lithium (Li) metal batteries employing solid polymer electrolytes. Extensive efforts have been devoted to tackling the crucial shorting problem in cycled polymer electrolytes via tuning the polymer chemistries and polymer–metal interfacial properties. However, the working principles of these designs mainly focus on physical/chemical suppression, instead of full recovery of the grown dendrites. Here, we propose an effective gradient design in polymer electrolytes by introducing Ga-based liquid metal (LM) particles with a depth-dependent content, enabling effective recovery of Li dendrites via spontaneous alloying reaction. Such an asymmetric electrolyte configuration is capable of fully chemically alloying the dendrites upon their puncturing into the LM-rich layer, while inhibiting electrical percolation at the LM-free layer, especially under mechanical pressure during cell assembly. Post-mortem analyses reveal the structural deformation of piercing dendrites into spherical Li–LM alloys, thereby preventing shorting even with extended cycles. Consequently, ultrastable cycling stabilities are achieved in both symmetric cells (>2000 h) and Li/LiFePO 4 full cells (>400 cycles; average CE of 99.86%). These findings not only exploit dendrite recovery functionality by using LM-based gradient electrolytes but also highlight the potential of incorporating gradient designs in various battery systems.

Solar-driven atmospheric water harvesting (AWH) presents a sustainable approach for freshwater production with sunlight as the sole energy input. To address challenges posed by diurnal moisture variations and diffusive sunlight, we present a system-wide approach that synergistically enhances moisture capture and solar energy utilization in an integrated water harvester. Moisture utilization at the bulk sorbent scale is improved through the hierarchical pore structure of scalable biomass gel sheets enabling rapid regeneration and is further upscaled to system-level performance through a kinetics-matched, continuously multicyclic operation protocol in a multilayered device. Solar energy utilization is enhanced by thermoresponsive hydrogels that lower the energy threshold for water desorption and by efficient thermal and mass flow management that increases energy efficiency. Our system delivers up to 235.09 mL d −1 of water with an energy efficiency as high as 26.4%, excluding solar panel power. This work offers an insight into developing energy-, material-, and space-efficient AWH systems from a cross-scale understanding of sorbent properties, device engineering, and operation protocol tailoring.

Abstract Aluminum–sulfur (Al–S) batteries catalysts with adsorption and catalytic capabilities can effectively improve the slow redox kinetics, but the current research often ignores the effect of optimizing the electronic structure of the catalyst on improving charge transfer and adsorption. Here, Ni‐doped monolayer MoS 2 nanosheets are synthesized and used as a catalytic additive for the sulfur cathode. The addition of Ni promotes spin splitting of 4d orbital of Mo, thereby affecting polarization degree of the basal plane sulfur and making it change from a low spin state to a high spin one. This high spin configuration raises the electron energy level and provides an active electron state to react with aluminum polysulfides (AlPSs), which optimizes the adsorption energy. At the same time, it accelerates electron transfer and lowers the energy barrier for the overall conversion of the polysulfides. Benefiting from these features, Al–S batteries based on rationally designed S@Ni‐MoS 2 /C cathodes exhibit a high initial capacity (1603.0 mAh g −1 at 0.5 A g −1 ) and extraordinary cycling stability (0.035% capacity decay rate during 2000 cycles). This study showcases a spin‐polarized electronic structure control strategy to enhance catalytic activity, providing a viable approach for developing efficient catalysts for practical Al–S batteries.

Abstract Aluminum–sulfur (Al–S) batteries catalysts with adsorption and catalytic capabilities can effectively improve the slow redox kinetics, but the current research often ignores the effect of optimizing the electronic structure of the catalyst on improving charge transfer and adsorption. Here, Ni‐doped monolayer MoS 2 nanosheets are synthesized and used as a catalytic additive for the sulfur cathode. The addition of Ni promotes spin splitting of 4d orbital of Mo, thereby affecting polarization degree of the basal plane sulfur and making it change from a low spin state to a high spin one. This high spin configuration raises the electron energy level and provides an active electron state to react with aluminum polysulfides (AlPSs), which optimizes the adsorption energy. At the same time, it accelerates electron transfer and lowers the energy barrier for the overall conversion of the polysulfides. Benefiting from these features, Al–S batteries based on rationally designed S@Ni‐MoS 2 /C cathodes exhibit a high initial capacity (1603.0 mAh g −1 at 0.5 A g −1 ) and extraordinary cycling stability (0.035% capacity decay rate during 2000 cycles). This study showcases a spin‐polarized electronic structure control strategy to enhance catalytic activity, providing a viable approach for developing efficient catalysts for practical Al–S batteries.

ABSTRACT The growing global population, coupled with increasing food demand and water scarcity, has intensified the need for advancements in modern agriculture. As an emerging class of materials featured by intensively tunable properties, smart hydrogels offer innovative solutions to challenges associated with conventional agricultural practices, such as excessive agrochemical and water use and inefficiencies that contribute to environmental degradation. Additionally, hydrogel‐based sensors can monitor environmental conditions and crop health, enabling precise adjustments to optimize growth and resource use. By serving as platforms for the slow and controlled delivery of agrochemicals and smart sensors, hydrogel systems can enhance resource efficiency, reduce labor demands, and improve crop yields in an environmentally sustainable manner. This Perspective article summarizes recent advancements in hydrogel‐based materials, highlights existing challenges, and proposes potential research directions, with a focus on developing advanced hydrogel systems to transform agricultural practices. image

The inter-site distance effect (ISDE) has gained significant attention in heterogeneous catalysis, challenging classical models that treat adjacent nonbonded sites as isolated. Recent studies demonstrate that these sites can exhibit long-range cooperative interactions, enhancing reaction efficiencies. Fully leveraging the ISDE to overcome limitations in site reactivity requires a multidisciplinary approach and advanced techniques. This review provides a comprehensive overview of ISDE in electrocatalysis, starting with strategies for synthesizing materials with tunable inter-site distances. It examines ISDE across various catalyst models, including monometallic and heteronuclear atomic sites, active sites within clusters, and the lattice of nanocatalysts, focusing on their electronic structures, spatial geometries, and synergistic interactions. Advanced characterization and computational methods are highlighted as essential for identifying inter-site structures and distances, providing a systematic framework for understanding ISDE's role in electrocatalysis. The review also proposes best practices for studying ISDE, addressing current challenges and offering future perspectives. These insights aim to inform the design of highly efficient catalysts, enhance the understanding of catalytic mechanisms, and contribute to the development of more efficient energy conversion technologies, providing a foundation for further research into optimizing electrocatalysts.

Abstract The inter‐site distance effect (ISDE) has gained significant attention in heterogeneous catalysis, challenging classical models that treat adjacent nonbonded sites as isolated. Recent studies demonstrate that these sites can exhibit long‐range cooperative interactions, enhancing reaction efficiencies. Fully leveraging the ISDE to overcome limitations in site reactivity requires a multidisciplinary approach and advanced techniques. This review provides a comprehensive overview of ISDE in electrocatalysis, starting with strategies for synthesizing materials with tunable inter‐site distances. It examines ISDE across various catalyst models, including monometallic and heteronuclear atomic sites, active sites within clusters, and the lattice of nanocatalysts, focusing on their electronic structures, spatial geometries, and synergistic interactions. Advanced characterization and computational methods are highlighted as essential for identifying inter‐site structures and distances, providing a systematic framework for understanding ISDE's role in electrocatalysis. The review also proposes best practices for studying ISDE, addressing current challenges and offering future perspectives. These insights aim to inform the design of highly efficient catalysts, enhance the understanding of catalytic mechanisms, and contribute to the development of more efficient energy conversion technologies, providing a foundation for further research into optimizing electrocatalysts.

Developing renewable energy and achieving decarbonization of energy systems is an inevitable trend. Flow batteries (FBs) have great potential in the field of large-scale energy storage due to their unique features of decoupled energy and power rating, scalability, and long lifetime. In this chapter, we summarize the state-of-art progress on the key components of FBs, including electrolytes (from classic inorganic to organic active materials), membranes, electrodes, and bipolar plates. Some novel FB technologies and industrial applications are also presented. Finally, the current challenges and perspectives on the exploration of high-performance FBs are also highlighted.

Abstract Atmospheric water harvesting (AWH) offers a promising pathway to alleviate global water scarcity, highlighting the need for environmentally responsible sorbent materials. In this context, this research introduces a universal strategy for transforming natural polysaccharides into effective hydrogel sorbents, demonstrated with cellulose, starch, and chitosan. The methodology unites alkylation to graft thermoresponsive groups, thereby enhancing water processability and enabling energy‐efficient water release at lower temperatures, with the integration of zwitterionic groups to ensure stable and effective water sorption. The molecularly functionalized cellulose hydrogel, exemplifying our approach, shows favorable water uptake of 0.86–1.32 g g −1 at 15–30% relative humidity (RH), along with efficient desorption, releasing 95% of captured water at 60 °C. Outdoor tests highlight the water production rate of up to 14.19 kg kg −1 day −1 by electrical heating. The proposed molecular engineering methodology, which expands the range of raw materials by leveraging abundant biomass feedstock, has the potential to advance sorbent production and scalable AWH technologies, contributing to sustainable solutions.

With the growing emphasis on building a global sustainable community, biopolymeric gels have emerged as a promising platform for environmentally friendly and sustainable applications, garnering significant research attention. Compared to conventional synthetic gels, biopolymeric gels offer numerous advantages, including abundant and renewable raw materials, energy-efficient and eco-friendly fabrication processes, tunable physicochemical properties, and superior biocompatibility and biodegradability. This review provides a comprehensive overview of recent advancements in multifunctional biopolymeric gels. It begins by introducing various biopolymeric building blocks and their intrinsic properties across multiple scales. Subsequently, the synthetic strategies for biopolymeric gels are thoroughly discussed, emphasizing versatile gelation strategies, multiple approaches for fabricating gels, diverse processing approaches to achieve tailorable gels with desired functionalities. The sustainable applications of biopolymeric gels are systematically explored, focusing on their roles in energy storage, environmental remediation of water management, thermal management, and bioelectronics. Finally, the review concludes with an outlook on the challenges and opportunities for advancing biopolymeric gels as key materials in the pursuit of sustainability.

Paring seawater electrolyte with zinc metal electrode has emerged as one of the most sustainable alternative solutions for offshore stationary energy storages owing to the intrinsic safety, extremely low cost, and unlimited water source. However, it remains a substantial challenge to stabilize zinc metal negative electrode in seawater electrolyte, given the presence of chloride ions and complex cations in seawater. Here, we reveal that chloride pitting initiates negative electrode corrosion and aggravates dendritic deposition, causing rapid battery failure. We then report a charge gradient negative electrode interface design that eliminates chloride-induced corrosion and enables a sustainable zinc plating/stripping performance beyond 1300 h in natural seawater electrolyte at 1 mA cm-2/1 mAh cm-2. The gradually strengthened negative charges formed via diffusion-controlled electrostatic complexation of biomass-derived polysaccharides serve to repel the unfavorable accumulation of chloride ions while simultaneously accelerating the diffusion of zinc ions. The seawater-based Zn | |NaV3O8·7H2O cell delivers an initial areal discharge capacity of 5 mAh cm-2 and operates over 500 cycles at 500 mA g-1. Seawater electrolytes provide a sustainable option for aqueous zinc batteries but challenge the stability of zinc metal electrodes. Here, authors elucidate the zinc electrode failure mechanisms and propose a charge gradient interface strategy to stabilize the zinc electrode in seawater electrolytes.

With the increasing popularity of electric transportation over the past several years, fast-charging lithium-ion batteries are highly demanded for shortening electric vehicles’ charging time. Extensive efforts have been made on material development and electrode engineering; however, few of them are scalable and cost-effective enough to be potentially incorporated into the current battery production. Here, we propose a facile magnetic templating method for preparing LiFePO 4 (LFP) cathodes with vertically aligned graphene sheets to realize fast-charging properties at a practical loading of 20 mg cm –2 . Graphene sheets decorated with Fe 3 O 4 nanoparticles can be responsive to an external magnetic field and can maintain their vertical alignment during the electrode fabrication process. The vertically aligned graphene provides the magnetized LFP electrodes (m-LFP) with simultaneously improved electron and lithium-ion transport properties, achieving 110 and 76 mA h g –1 at 3C and 4C, respectively. Furthermore, magnetized Fe 3 O 4 (m-Fe 3 O 4 ) anodes were also prepared via the magnetic templating method to vertically align the Fe 3 O 4 nanosheets inside, which outperforms the conventional graphite anodes at a high rate of 3C. Finally, by pairing the magnetized LFP cathode and Fe 3 O 4 anode, we demonstrate the simultaneous fast-charging properties and good cycling stability in the m-LFP||Fe 3 O 4 full cells. This study not only provides an effective methodology for achieving vertically aligned structures which can potentially be incorporated into industrial manufacturing but also brings insightful considerations for designing scalable fast-charging energy storage systems.

Liquid metals (LMs), i.e., metals and alloys that exist in a liquid state at room temperature, have recently attracted considerable attention owing to their electronic and rheological properties useful in various cutting-edge technologies. In this study, eutectic Ga–In (EGaIn), one of the most studied LMs, in its microdroplet form was engineered to produce a novel droplet-type surfactant that can stabilize a liquid- in -liquid emulsion with unique functionality and processability. Dual-engineered LM droplets with a robust SiO 2 encapsulation shell and adsorbed amphiphilic cetyltrimethylammonium bromide (CTAB) exhibited high chemical stability against water-mediated oxidation while possessing excellent oil–water interfacial activity. These engineered droplet-type surfactants densely adsorb at microscale water–oil interfaces and prevent coalescence of the dispersed oil droplets in the liquid continuous phase, thereby producing long-term stable oil- in -water (O/W) emulsions─these droplet-type surfactants were named as “mutant” Pickering emulsifiers, indicating particle emulsifiers (different from molecular surfactants) that are similar to conventional Pickering emulsifiers, but consisting of the liquid core instead of the solid . The resulting emulsions exhibited enhanced yield stresses with viscoelastic properties, even at a minimal LM load, and showed remarkable sedimentation stability, indicating significant implications in terms of processability in versatile applications. The “structured” nature of such emulsions combined with the excellent photothermal conversion ability of LM droplets adsorbed at O/W interfaces resulted in the extremely localized photothermal heating effect. Furthermore, photothermally responsive phase-change oil droplets were produced using engineered LM droplets, which can be used for the on-demand release of valuable oil-soluble cargo as a potential application. We expect that engineered LM droplets as novel droplet-type emulsifiers of immiscible liquids in colloidal multidisperse systems will provide unique opportunities for various applications.