Harvesting solar thermal energy in the mid-temperature (80-90 degrees C) through phase change materials (PCMs) is a promising carbon-neutral pathway for affordable and sustainable energy storage. However, they face considerable issues with supercooling, phase separation, and poor thermal conductivity. To overcome these issues, a novel, form-stable and durable composite PCM based on aluminum potassium sulfate dodecahydrate (APSD) was developed. The incorporation of 2 wt% magnesium chloride hexahydrate (MCH) as a nucleating agent significantly reduced the supercooling from 32.86 degrees C to 17.04 degrees C. Furthermore, the composite PCM modification with sodium lignosulfonate (SL), which working as a sustainable and multi-functional thickening agent, effectively suppressed phase separation and enhanced the enthalpy by 12.0%. The APSD-MCH-SL composite presented a stable phase change temperature (84.96 degrees C), high enthalpy (251.0 J/g) and no phase separation. Subsequently, expanded graphite (EG) was introduced as scaffold and thermal conductive bridge to fabricate a form-stable and durable APSD-MCH-SL/EG composite, which retained a melting point of 81.66 degrees C, a high enthalpy of 224.4 J/g and an improved thermal conductivity of 0.461 W/(m.K). Notably, the SL was acted as a compatibilizer enhanced interaction of EG network to the APSD hydrate and helped to mitigate liquid leakage. Overall, the composite PCMs present an exciting combination of cost-effective hydrated salts and functional lignin materials that demonstrate a reliable and efficient approach for solar thermal energy storage.

Abstract The rational design of materials with tunable compositions remains challenging due to the vastness of compositional space. Herein, we propose a genome-inspired materials intelligence framework (GIMI) for inverse design in high-dimensional compositional spaces. By integrating a multi-estimator disagreement-based data filtering strategy with a genetic algorithm, this framework enables on-the-fly improvement of the machine-learning predictive accuracy and efficient exploration of diverse compositions, thereby significantly enhancing search efficiency while reducing computational cost. Applied to graphene-based single-atom catalysts (SACs) with variable ligands for CO2 electroreduction to CO, GIMI efficiently screens 34,992 possible metal-ligand combinations and identifies promising SACs (e.g., Zn-O1N3 and Zn-O2N2) by evaluating only ∼1250 structures per round, demonstrating its high search efficiency. Further interpretability analysis reveals that the cohesive energy and electronegativity of the metal center primarily govern CO2RR activity, while ligands play a secondary role by modulating the local coordination geometry. This work establishes a scalable and generalizable platform for inverse materials design, enabling targeted exploration of complex compositional space and accelerating the discovery of high-performance catalysts.

Developing anode catalysts that can reduce the utilization of iridium noble metal, one state-of-art catalyst for acidic water oxidation, while maintaining high catalytic activity and stability is of crucial significance for the advancement of proton exchange membrane water electrolyzer (PEMWE). In this study, we present iridium-platinum oxide solid solution nanoparticles (IrPtOx) supported on commercial rutile TiO2 with 45 wt% Ir content for oxygen evolution reaction (OER), reducing the Ir loading to 0.18 mgIr/cm2 in PEMWE. Epitaxial growth of platinum oxides layer onto TiO2 facilitates the active species generation in the following Ir integration by molten salt process. We evidence that an optimized charge redistribution between Ir and Pt in the IrPtOx alters the predominant OER mechanism to enhance dual activity and stability, incorporating the adsorbate evolution mechanism (AEM) with the lattice oxygen mechanism (LOM). Notably, the assembled device achieves a current density of 1 A/cm2 at a cell voltage of 1.66 V and good durability over 270 h.

The development of flexible wearable electronics (FWE) that integrate high sensitivity, excellent strain tolerance, and multi-signal decoupling capability is of great significance, yet remains challenging. Herein, a rigid-flexible supramolecular unit is constructed by incorporating flexible demethylated lignin (DL) onto the surface of rigid cellulose nanofibers (CNF) framework (DL@CNF). This supramolecular unit integrates high-strength rigid load-bearing with a high-efficiency energy dissipation mechanism at the nanoscale, which confers high fatigue resistance and stable signal transmission. The presence of rigid crystalline regions and the sufficient dynamic interaction sites on the DL@CNF endow the eutectogel with superior mechanical properties (approximate to 343 kPa, 5000%), robust adhesion (approximate to 110 kPa), good self-healing property, and excellent UV shielding capability (99.5%). Benefiting from the above integrated features, the wearable sensors that harness the eutectogel as the generation of high-fidelity electrical signals in response to strain, pressure, and temperature over a broad temperature range (-80 degrees C to 60 degrees C). This work unlocks immense potential as a generic platform for biomass-derived supramolecular engineering, offering a unique opportunity to create tailored materials for advanced bio-based flexible electronics.

Solar-driven water splitting provides a clean and essential pathway to green hydrogen for future, sustainable energy systems. Among the developed photocatalytic materials, inorganic semiconductors are particularly attractive because of their earth abundance, scalable synthesis, and potential for high-energy conversion efficiency. Prototypical Ti-based oxide single crystals, such as TiO2 and SrTiO3, have been extensively investigated as model photocatalysts, owing to their well-defined electronic structures and excellent chemical stability. However, two fundamental limitations remain: the inefficient separation and migration of photogenerated charge carriers, and the spatial colocalization of hydrogen and oxygen evolution sites. Together, these factors lead to severe charge recombination and promote back-reactions, thereby substantially constraining the overall efficiency of photocatalytic water splitting.Long-standing efforts in this field have consistently highlighted facet engineering as a powerful means of overcoming these critical limitations. Facet-dependent modulation imparts crystallographic anisotropy directly to the key functional attributes of the photocatalyst, manifesting as directional enhancements in charge separation efficiency and interfacial reaction kinetics. In this regard, facet-specific atomic electronic engineering induces internal electric fields that direct charge migration and isolate redox sites, therefore boosting photocatalytic water splitting.In this Account, we provide a comprehensive review of our group's progress over the past two decades in controlling anisotropic facets in Ti-based oxides. By developing a suite of controllable synthetic strategies based on liquid-phase and solid-state routes, we demonstrate, guided by Wulff theory, that inorganic ions and organic small molecules can systematically modulate the surface energies of specific crystal facets, thereby enabling rational, theory-informed facet engineering. We have established a series of strategies for preparing single-crystalline TiO2 and SrTiO3 with well-defined anisotropic surface structures. These efforts have deepened our understanding of the intrinsic structure-activity relationships that connect crystallographic architecture to photocatalytic performance. We highlight how advances in characterization techniques in recent years have greatly sharpened our understanding of facet-dependent charge transport and surface reaction kinetics. We anticipate that these insights will provide a robust foundation for future developments in the field, including the rational design of facet-specific catalysts, detailed elucidation of interfacial reaction mechanisms, and the coordinated integration of multiscale theoretical and experimental approaches. A more explicit link between structure and function is expected to play a decisive role in guiding the development of high-efficiency photocatalytic systems and in accelerating the practical implementation of solar-driven hydrogen production.

Single-atom co-catalysts engineered on semiconductor substrates offer a cost-efficient pathway to improve the photocatalytic performance with minimal precious metal loading. However, the precise tuning of local coordination environments and the construction of efficient single-atom co-catalysts remain challenging for photocatalytic overall water splitting systems. In this work, we have employed an icing-assisted photochemical reduction strategy to anchor atomically dispersed Pt species as hydrogen evolution co-catalysts on Al3+-doped SrTiO3 (Pt SA-STO) for photocatalytic overall water splitting. The optimized Pt SA-STO exhibits remarkable photocatalytic performance, achieving hydrogen and oxygen evolution rates of 13.62 and 6.71 mmol h−1 g−1, respectively, along with a turnover frequency (TOF) value of 2114.5 h−1. We pioneer the application of nuclear magnetic resonance (NMR) spectroscopy to quantitatively characterize the temporal evolution of Pt4+ to Pt2+ under continuous irradiation during the icing-assisted photoreduction process; besides, advanced characterizations and theoretical calculations well evidence that single-atom Pt co-catalysts facilitate directional transfer and extraction of photogenerated charge carriers, effectively suppressing surface recombination of photogenerated electron-hole pairs. This work offers valuable insights into the design of novel single-atom co-catalysts by deepening the understanding of electronic configurations and active sites in photocatalytic overall water splitting.

Glasses made from organic-inorganic hybrid perovskites are emerging non-crystalline semiconducting materials whose versatile composition and exceptional processability allow for manifold applications. The current melt-quenching approaches are compatible to only few perovskite crystals, as most undergo irreversible decomposition prior to melting. Herein, we report a general flux-mediated approach to produce a library of high-quality perovskite glasses with different organic molecules, metal centers, and framework dimensionality. We show that the partial deprotonation of organic moiety by alkali metal hydroxide flux modulates the intermolecular interactions in perovskites, and activates the flow unit, which depresses the fusion temperature ranging 21–77 °C with flux ratio <1.1 wt%. More critically, the utilization of hydroxide flux creates a large melt window, and enables the thermal vitrification of many inherently non-meltable systems, such as (BA)2PbI4 (BA = butylamine) and (DGA)PbI4 (DGA = 1,1-dimethylbiguanide). Using these semiconductive glasses, we realize high-performance X-ray detection devices showing a sensitivity of 35674.1 μC Gyair−1 cm−2 under 500 V mm−1 electric field, and a high-resolution X-ray imaging system via its seamless integration on commercial thin-film transistor backplanes. The discovery of hybrid perovskite glasses opens new opportunities for tailoring the properties of semiconducting materials. Wang et al. report a flux-mediated approach for synthesizing a family of perovskite glasses with varied organic constituents while lowering fusion temperatures through deprotonation.

Designing ruthenium (Ru)-based catalysts for the acidic oxygen evolution reaction (OER) remains highly challenging due to the intrinsic instability of the Ru active site. Anchoring the Ru site on other metal oxides is a widely used strategy. To elucidate how metal-oxide substrates influence the performance of anchored Ru sites under acidic OER, we established a screening framework to identify the potential metal oxides (e.g., rutile-, spinel-, pyrochlore- and perovskite-type) by density functional theory calculations and discussed the substrate-dependence of the anchored Ru active site. Applying a set of predetermined criteria, we screened 39 promising candidates, including 11 rutile-, 14 spinel- and 14 pyrochlore-type metal oxides, from 1513 metal oxides in the Materials Project Database, which could be suitable for stabilizing the Ru active center. Perovskite-type metal oxides are unsuitable due to their unstable structural framework with weaker metal-oxygen bonds. The rutile-, spinel- and pyrochlore-type metal oxide substrates can break the linear scaling relationships between the key OER intermediates on the Ru site; especially, spinel- and pyrochlore-type oxides exhibit a smaller slope in this relationship, indicating a stronger substrate effect and their greater potential as platforms for designing Ru-based catalysts. This work provides guidance for the experimental discovery of suitable metal oxide substrates for constructing Ru-based catalysts for the OER and offers fundamental insights into the substrate-dependent behavior of the Ru site on different metal oxides.

CO2 conversion in proton exchange membrane (PEM) electrolysis systems offers a sustainable pathway for chemical production by eliminating carbonate formation; however, it faces a trade-off between suppressing the hydrogen evolution reaction and preventing salt precipitation. Here, we resolve this paradox through a molecular-level engineering strategy by anchoring a mercaptoimidazole ligand on lead-based catalyst. Operando spectroscopic analyses and theoretical studies reveal that this ligand shell creates a local alkaline microenvironment and establishes a proton-shielding effect at the catalyst surface. When integrated into a zero-gap PEM electrolyzer, the catalyst achieves a peak formate Faradaic efficiency of 95.8% and sustains over 90% selectivity at a current density of 600 mA cm-2. This performance persists under strongly acidic (pH 1.0) and cation-starved (0.001 M) conditions. The PEM system delivers extended stability, with over 300 h of continuous operation at industrially relevant current densities. Our work establishes a design strategy that decouples the catalytic microenvironment from the bulk electrolyte and provides a route for durable and selective acidic CO2 electrolyzers.

Coupling the glycerol oxidation reaction (GOR) with hydrogen production offers significantly higher energy efficiency for the electrosynthesis of value-added chemicals compared to the sluggish oxygen evolution reaction (OER). However, developing low-cost electrocatalysts for high-efficiency GOR remains challenging due to the absence of strategies to stabilize active species while efficiently facilitating the conversion of glycerol at industry-level current densities. Herein, a Fe-doped cobalt hydroxide electrocatalyst for GOR is reported, which achieves 700 mA cm-2 at a voltage of 1.46 V vs. RHE, meanwhile showing formate Faradaic efficiency around 90 % and excellent stability (144 h at 1.40 V vs. RHE). The coupled GOR//HER system in the membrane electrode assembly merely requires 2.05 V to sustain a current density of 1 A cm-2, maintaining stable operation for 120 h. In situ Raman spectroscopy and theoretical analysis reveal that Fe doping preserves CoOOH from dehydrogenation to CoO2, which acts as a stable and active site for facilitating the rate-determining step of glycerol dehydrogenation and the C-C bond cleavage in GOR. This work presents an innovative perspective on elucidating the reaction mechanism of cobalt-based catalysts in GOR, proposes the effect of the dehydrogenation capacity of active sites on catalytic performance, and offers valuable guidance for optimizing catalyst design.

Acid precipitation is a widely adopted method for lignin recovery from pulping black liquor, where the precipitation parameters determine the structural and physicochemical characteristics of the isolated lignin. Given the structural complexity and heterogeneity of lignin, the impact of acid type on its molecular structure and surface chemistry remains unclear. This study investigates how differences in protonation kinetics among various acids influence lignin particle morphology and their interfacial behavior in cellulose composite films. The results indicate that lignin precipitated using HCl forms spherical particles with size (190 +/- 51.1 nm), good monodispersity (PDI = 0.072) and long-term aqueous stability. This is attributed to the strong acidity of HCl, which enables rapid H+ release and complete protonation of lignin molecules. Conversely, the weaker acidity of ethanoic acid (HAc) leads to a more gradual protonation, resulting in hierarchically structured particle aggregates with a broader size distribution (240 +/- 111.6 nm, with many nanoparticles < 50 nm). In addition, HCl-lignin and HAc-lignin composite films showed 38.4% and 39.3% increases in elongation at break over pure cellulose films, along with substantial UV-blocking efficiency enhancements of 540% and 745%.

Polyethylene terephthalate (PET) can be electrochemically upgraded into value-added chemicals under mild conditions, providing a viable strategy for the coupled aims of plastic-waste valorization and decarbonization. Replacing the anodic oxygen evolution reaction (OER) with PET-derived ethylene glycol electrooxidation reaction (EGOR) markedly reduces the required cell voltage while co-producing H2 and value-added products. However, realizing these applications hinges on the design of efficient and stable catalysts that enable selective oxidation. Herein, we demonstrate a novel EGOR pre-catalyst, Cl- doped cobalt hydroxide on a Ni foam (NF) substrate (Co(OH)2-Cl/NF), which undergoes chlorine etching through electrochemical activation, inducing the gradual in situ reconstruction of the pre-catalyst into a highly active EGOR catalyst (CoOOH-VCl/NF). During EGOR, CoOOH-VCl/NF demonstrates a current density of 400 mA cm-2 at 1.37 V versus RHE, alongside a Faradaic efficiency of 96.9% for formate generation, while retaining stable performance over 100 h of uninterrupted operation, thus underscoring its considerable industrial application potential. The "Cl- etching-induced material dynamic reconstruction" strategy proposed in this work not only provides a novel approach for constructing highly efficient EGOR electrocatalysts, but also lays the foundation for synergistically advancing the high-value utilization of plastic waste and green hydrogen production.

Perovskite single crystal arrays combine the advantages of low defect density, coherent lattice orientation and multiplexed channels, which offer great potential across various fields ranging from energy conversion and signal detection to flexible electronics. However, the poor regularity in the morphology, composition, and heterophase of perovskite arrays poses a major challenge in manipulating the optical and electronic characteristics. Here, we demonstrate a non-invasive general epitaxial growth approach for fabricating perovskite single-crystalline heterostructure arrays with programmable dimensions, geometry, and composition on various substrates. The solvation structure during array epitaxy is meticulously manipulated by co-solvents, which minimizes the detrimental nucleus dissolution and favors the formation of well-defined and uniform perovskite heterostructure arrays. The electronic properties of the fabricated perovskite arrays approach those of bulk single crystals with a carrier mobility of 18.29 cm2 V- 1 s-1 and a trap density of 5.76 × 1012 cm-3. Using these heterostructure arrays, micro-LED devices have been fabricated exhibiting unique electrochromic function. The programmable production of perovskite heterostructure arrays offers a well-defined platform for fundamental studies and device integration of perovskite-based optoelectronics.

To address plastic pollution and food preservation challenges through the valorization of industrial by-products, we developed a high-performance food packaging film incorporating beeswax and sodium lignosulfonate (LS). In this system, LS served a dual function: as a submicron emulsion stabilizer, it enabled the formation of a stable and uniform dispersion of hydrophobic beeswax, and as an interfacial compatibilizer, it strengthened adhesion between the cellulose matrix and the wax phase within the composite film. This synergistic design produced a film with a tensile strength of 107 MPa, representing a 133% increase over pure cellulose, along with exceptional barrier properties, including an oxygen permeability (OP) of 1.95 cm3 center dot & micro;m center dot m-2 center dot day-1 center dot kPa-1 and a water vapor permeability (WVP) of 6.98 & times; 10 3 g center dot & micro;m center dot m-2 center dot day-1 center dot kPa-1 , while maintaining high visible light transmittance (87%). The lignin incorporation also conferred antioxidant and antibacterial functionalities to the films and effectively extended the shelf life of cherry tomatoes under normal storage conditions. This design successfully reconciles the trade-off between in-use durability, as predicted by Arrhenius modeling, and rapid end-of-life biodegradability, providing a versatile blueprint for next-generation, circular bio-based packaging materials.

Metal halide perovskites are promising candidates for low‐cost and sensitive x‐ray detection. However, the existing perovskite materials with diverse composition and dimensionality encounter an intrinsictrade‐off between carrier collection and ion migration, posing a critical challenge for high‐energy x‐ray detection. Here, we demonstrated that the quasi‐one‐dimensional perovskite of cystamine lead iodide featuring corner‐sharing [Pb 5 I 22 ] chains chain and small interchain spacing along edge‐on orientation enables efficient carrier collection and blocked ion migration simultaneously, and thus largely decouple the electronic and ionic transport pathways. The as‐grown single crystals yield a large mobility‐lifetime product of 4.35 × 10 −4 cm 2 V −1 , and a high activation energy for ion migration of 0.94 eV. Therefore, an impressive x‐ray sensitivity of 1.42 × 10 5 µC Gy −1 cm −2 (average x‐ray energy 42.7 keV) are obtained in quasi‐one‐dimensional perovskite. Under harsh conditions, such as continuous radiation, high electric fields, and high temperatures, the device exhibits excellent operational stability. As a proof of concept, the robust integration of a quasi‐one‐dimensional perovskite with a thin‐film transistor backplane for x‐ray imaging was achieved. This study offers innovative insights into the regulate the structural dimensions of materials for sensitive and stable x‐ray detection.

ABSTRACT The development of noble‐metal‐free cocatalysts is crucial for low‐cost photocatalytic overall water splitting (POWS) systems. However, dynamic structural evolution of non‐noble‐metal materials under operando conditions results in a restricted activity of cocatalysts in POWS. Herein, we construct a core–shell structured Cu@Cr 2 O 3 cocatalyst on Al‐doped SrTiO 3 (SrTiO 3 :Al) via a photodeposition method (denoted as Cu‐PD/STO) for efficient H 2 evolution in POWS. The Cu‐PD/STO achieves the H 2 evolution rate of 788.7 µmol/h, surpassing all the recently reported noble‐metal‐free H 2 evolution cocatalysts on SrTiO 3 for POWS. Quasi in situ/ operando characterizations elucidate the stable operation of Cu 0 active sites in POWS, guaranteed by the photoinduced reduction of Cu sites and core–shell structure. Further characterizations and theoretical calculations reveal that Cu 0 active sites provide accelerated electron extraction from SrTiO 3 :Al, optimized water dissociation, and hydrogen adsorption. Moreover, Cu 0 active sites can promote the formation of Cr 2 O 3 shells, which encapsulate the Cu 0 active sites, protecting them against surface oxidation and suppressing the reverse reaction in POWS.

Low-dimensional hybrid metal halides (HMHs) are promising for next-generation optoelectronics due to their structural diversity and excellent photophysical properties. However, weak ionic interaction and electronic coupling between organic-inorganic moieties lead to structural instability and inferior carrier transport. Here, we report one-dimensional hybrid lead halide crystals using multidentate aminoazole molecules that form Pb-N coordination bonds at the organic-inorganic interface. This dual-side bonding locks the hybrid structure, hinders ion migration, and promotes charge transport through electronic orbital overlap. An X-ray detector based on ATDZPbBr3 polycrystalline wafers achieves the highest sensitivity of 1.63 × 104 μC Gyair-1 cm-2 and an ultralow detection limit of 19.7 nGy s-1. This work establishes coordination chemistry as a powerful design paradigm for stable, high-performance hybrid semiconductors.

Among various hydrogen production technologies, proton exchange membrane water electrolysis (PEMWE) shows significant potential due to its high efficiency and flexibility. However, its large-scale application is limited by the reliance on precious metals. Herein, we report the successful uniform doping of titanium (Ti) into iridium oxide (IrOx) through an organic ligand complexation strategy, obtaining a sub-2 nm Ti-doped IrOx (sub-Ti-IrOx) for stable oxygen evolution reaction in acid. Doped Ti regulates the Ir–O bond length to facilitate the formation of key intermediates, while also acting as an electron donor to suppress the over-oxidation of IrOx, thereby enhancing both catalytic activity and stability. The ultra-small particles offer a larger electrochemical active surface area and facilitate good dispersion during the membrane electrode assembly fabrication, enabling the formation of a catalyst layer with highly uniform thickness. When incorporated into a proton exchange membrane electrolyzer, sub-Ti-IrOx exhibits a current density of 1 A cm−2 at a voltage of 1.667 V and maintains stable operation for over 600 h with a voltage decay rate of approximately 33 μV h−1. This study confirms the effectiveness and feasibility of Ti doping in simultaneously enhancing both the activity and stability of Ir-based catalysts.

Photocatalytic conversion of biomass-derived platform molecules provides a promising route to store intermittent solar energy as clean chemical energy, enabling the sustainable production of high-value chemicals from abundant, low-cost biomass. However, achieving high selectivity and conversion efficiency remains challenging due to the inherent complexity of multistep interfacial reaction pathways. This review concludes recent advances in mechanistic investigations that encompass all crucial processes, including active species evolution, intermediate transformation, charge transfer, and chemical bond cleavage/reformation, employing advanced experimental methods, including electron paramagnetic resonance spectroscopy, radical quenching, isotope labeling, and in situ Fourier transform infrared spectroscopy. The applicability, sensitivity, and limitations of these techniques are critically evaluated across diverse reaction environments. Finally, we outline key challenges, such as limited temporal resolution, and discuss prospects for integrating complementary operando techniques with data-guided mechanistic modeling.

Agricultural and forestry residues have attracted increasing attention as promising alternatives to petroleum-based materials due to their abundance and renewability. This study developed a strategy based on the interplay of mechanical treatment and alkaline deep eutectic solvent (DES) for simultaneous preparation of lignin-containing cellulose nanofibrils (LCNF) and lignin nanoparticles from wheat straw. Initially, the wheat straw was mechanically fibrillated with mechanical refining to disrupt the hierarchical structure. Then, an alkaline DES system with a high hydrogen-bonding capacity composed of choline chloride (ChCl) and monoethanolamine (MEA) was employed to effectively deconstruct wheat straw which facilitated strong hydrogen bonding interactions with the biomass, promoting lignin removal efficiency. Under the optimized treatment conditions (ChCl: MEA = 1:8, 90 degrees C, 9 h), the delignification rate reached 81.61% while maintaining a cellulose retention rate of 92.08%. After solid-liquid separation, the solid fraction was further homogenized to obtain LCNF, which exhibited a high zeta potential (-17.30 mV) and excellent dispersion stability with the yield of LCNF reached 61.70%. Meanwhile, 81.81% of the beta-O-4 linkages was retained in the DES recovered lignin, which is favorable for formation of lignin nanoparticles. As a results, spherical lignin nanoparticles with an average diameter of 237.14 nm were isolated by dialysis, and the yield of lignin reached 20.50%. The process achieved a comprehensive utilization efficiency of 94.79% for wheat straw. The proposed strategy offers an efficient approach for the fractionation of wheat straw into lignin and nanocellulose functional materials.