Photocatalytic CO2 reduction requires catalysts to simultaneously coordinate two distinct half reactions: CO2 activation and H2O dissociation. However, most current materials lack electronically asymmetric sites capable of simultaneously driving both reactions efficiently. Herein, platinum (Pt) is introduced onto oxygen-vacancy (Ov)-rich InOOH to construct a novel interfacial Pt-Ov-In2+ Lewis pair via dynamic electron regulation, where Pt nanoparticles anchor oxygen vacancy and partially reduce adjacent In3+ to In2+, generating a charge-polarized region. Pt simultaneously modulates the Ov population via a reversible electronic interaction, maintaining an optimal balance of Pt-0 and the Ov-In2+ sites. Mechanistically, Pt functions as a Lewis-acid H2O activation site, accelerating O-H splitting, while Ov-In2+ serves as a Lewis-base center for CO2 adsorption and bending, stabilizing *CO2- and *CHO intermediates through strengthened In 5s/CO2 antibonding orbital interactions. As a result, Pt/InOOH-Ov delivers a CH4 formation rate of 227.2 mu mol g(-1) h(-1) with 99.0% selectivity, nearly 3 orders of magnitude higher than vacancy-rich InOOH. This work highlights Lewis-pair engineering across vacancy-rich oxide interfaces as a powerful strategy for multielectron CO2 conversion

Developing quantum dots (QDs) with robust and stable photoluminescence are critical for the advancement of optical nanomaterials. However, QD synthesis still usually involves complex nucleation, growth, surface capping, and separation procedures. Herein, we present an approach to generating embedded PbI2 QDs in situ within the matrix of a metal-organic framework (MOF) glass. This is achieved by controllable decomposition of an optoelectronically inactive delta-phase organic lead halide perovskite (OLHP) within the MOF glass, where the high-temperature MOF melt alters the degradation pathway through interfacial bonding and dissolution effects, effectively preventing PbI2 aggregation and passivating the resulting QDs. The resulting composite exhibits high-quality, narrow line width photoluminescence at room temperature, alongside remarkable stability under ambient conditions. This innovative approach offers a sustainable and efficient route for QD generation, underscoring the potential of MOF glass-based composites in optoelectronic applications.

Conventional hydrophobic membranes often suffer from fouling accumulation due to the absence of effective self-cleaning mechanisms, thereby hindering their long-term operational stability and recyclability. In this study, a polyacrylonitrile (PAN)-based composite nanofiber membrane with a hierarchical micro-nano surface structure was fabricated by combining the in-situ growth of TiO2 with an optimization of octadecyltrimethoxysilane (OTMS) coating morphology. Benefiting from the unique hierarchical morphology of micron-scale flower clusters and nano-protrusions, coupled with the synergistic effect of photocatalyst TiO2 and the superhydrophobic layer OTMS, the resulting nanofiber membrane (PAN/TiO2/OTMS) exhibited outstanding dual-functional properties of superhydrophobicity (water contact angle >154 degrees, sliding angle <5 degrees) and photocatalytic activity (a degradation efficiency of 99 % for methylene blue within 150 min). Moreover, the PAN/TiO2/OTMS nanofiber membrane demonstrated favorable demulsification capability in water-in-oil emulsions, with an oil permeation flux of 2388 L m(-2)& centerdot;h(-1) and a water separation efficiency of 99.9 %. More importantly, owing to dual self-cleaning mechanisms of physical superhydrophobicity and chemical photocatalysis, the as-prepared PAN/TiO2/OTMS exhibited a favorable antifouling and regeneration performance, demonstrating the oil flux recovery above 83 % and the irreversible fouling ratio below 17 % after multiple operation cycles. This study offers a practical strategy for the rational development of advanced membranes that integrate synergistic physical and chemical self-cleaning properties.

Amorphous metal-organic framework (MOF) glasses offer processible microporous materials for separation, sensing and catalysis, but their practical implementation has been limited by poor mechanical stability and ill-defined microporous structures. Here, we report a strategy to integrate g-C3N4 nanosheets into MOF glass via high-temperature sintering. Interfacial coupling, including π-π stacking and coordination-assisted bonding, effectively guides the packing of the nanosheets, improves structural integrity, and mitigates processing-induced stress during MOF glass vitrification. By tuning the sintering temperature, the interlayer spacing of the g-C3N4 can be adjusted and stabilized, generating more regulated transport channels. The resulting hybrid glass can be processed into membranes, showing a two-order-of-magnitude increase in hydrogen permeance compared to pure MOF glass, with the selectivity for difference gas pairs also significantly improved. This contribution establishes a generalizable method for interlayer spacing engineering within hybrid glasses, demonstrating that the incorporation of 2D materials can enhance the processability and separation performance of the composite glass.

Climate change has driven the development of sustainable catalytic processes to power our society. Applying solar energy to drive catalytic reactions is regarded as a green chemistry for value-added conversions. The photogenerated electrons have been applied for many promising processes such as hydrogen production, carbon dioxide reduction and nitrogen fixation, but the photogenerated holes are less focused on. Other than the traditional oxygen evolution reaction (OER), which has low economic value, some more promising reactions are expected to be explored, including water oxidation for hydrogen peroxide generation and methane oxidation for methanol generation. In this review, we will summarize the alternative partial water oxidation reaction (PWOR) and partial methane oxidation reaction (PMOR) for the production of useful hydrogen peroxide and methanol, respectively. Advanced materials engineering has been implemented to perform valuable conversions of photogenerated holes. The design concepts, principles, and traditional catalysts for PWOR and PMOR have been summarized. It is expected that this review will advance solar-driven reactions to another innovative stage with the aim of creating more value from photogenerated charges.

Electrochemical CO2 reduction is emerging as a compelling route for renewable energy storage and carbon neutrality. Focus on improving catalyst selectivity and energy efficiency resulted in a surge of catalysis-centered research. The advent of artificial intelligence and high-throughput screening enables parallelized catalyst characterization to accelerate discovery, but their implementation into application-relevant device configurations is challenging. We present a scalable, high-throughput platform based on infrared thermography that preserves realistic electrochemical environments from lab to industrially relevant scales. We demonstrate the spatial and electrochemical homogeneity of a 16-well parallel electrolyzer and validate a combinatorial testing approach using copper-based catalysts with varied loadings and precursor chemistries. The results highlight how activity trends can be rapidly mapped under controlled conditions, while also revealing the limitations of activity-only combinatorial testing, particularly for multiproduct electrochemical applications in complex environments like CO2 electrolysis on Cu. This platform thus provides an efficient pre-screening tool to accelerate catalyst discovery when analyzed appropriately and paired with follow-up single catalyst testing.

Hydrogen-bonded organic frameworks (HOFs) have emerged as promising porous materials for membrane fabrication. In this study, HOF-GS-10, synthesized from the dual ligands 1,5-naphthalenedisulfonic acid (providing sulfonic acid groups, -SO3H) and guanidine hydrochloride (providing guanidinium cations, -C (NH2)+3 ), was selected as a nanofiller to prepare high-performance thin-film nanocomposite (TFN) membranes for reverse osmosis (RO) desalination. The HOF-GS-10 nanoparticles were uniformly incorporated into the poly-amide (PA) active separation layer on a polysulfone (PSF) substrate via interfacial polymerization. Benefiting from the synergistic effects of the ultrathin PA layer, the porous structure of HOF-GS-10, and the strong hydrophilicity of the sulfonic acid groups, the resulting TFN membrane exhibited an average water permeability of 74.6 L center dot m-2 center dot h-1 center dot MPa-1, which is 260% of that the pristine thin-film composite (TFC) membrane that of the pristine thin-film composite (TFC) membrane, while maintaining a high NaCl rejection rate of 99.3%. Moreover, the HOF-modified TFN membrane demonstrated high desalination performance using natural seawater, achieving an average water permeability of 16.7 L center dot m-2 center dot h-1 center dot MPa-1. In addition, the membrane showed excellent antifouling performance against 500 ppm humic acid (HA), with a water flux recovery rate of 95.2%, and exhibited stable operation over 48 h. Molecular dynamics (MD) simulations revealed that the incorporation of hydrophilic HOF-GS-10 into the PA layer enhances water permeability by increasing the number of hydrogen-bonding sites available for water transport. This study not only proposes a novel strategy for developing highperformance RO membranes but also opens a new avenue for the application of HOF nanomaterials in advanced water treatment applications.

Metal–organic framework (MOF) glasses combine the processability of amorphous solids with molecular-scale porosity, yet they are made predominantly by melt-quenching, which requires high temperatures and fixes vitrification, shaping and pore formation in a single step. Here we report a sol–gel route that kinetically arrests zeolitic imidazolate framework (ZIF) coordination networks into metastable glassy states at room temperature, bypassing melt-quenching. This route is general: it spans zinc and cobalt centres, the ZIF-62 and ZIF-4 frameworks and a library of halogenated, methylated, amino-functionalised and sterically modified imidazolate linkers, reaching compositions not readily accessible by conventional melt-quenching synthesis. It also runs in low-cost alcohol solvents and scales to litre-sized reaction systems. Because the glass forms at room temperature, thermal relaxation can become an independent post-synthetic step that homogenises local coordination environments and redistributes free volume. This allows micropores to become narrower yet more connected and CO2 diffusivities to exceed those of melt-quenched glass by 5-fold. The sol or gel can be shaped into monoliths, films and thin composite membranes before the pore network is set, and such membranes surpass permeability–selectivity upper bounds for several gas pairs. Sol–gel chemistry thus turns structural relaxation into a synthetic handle for programming microporosity in coordination-network glasses.

Protonic ceramic fuel cells (PCFCs) are one of the promising routes to generate power efficiently from various fuels at economically viable temperatures (500-700 °C) due to the use of fast proton conducting oxides as electrolytes. However, the power density and durability of the PCFCs are still limited by their cathodes mostly made from solid metal oxides, which are challenging to address the sluggish oxygen reduction reaction and susceptibility to CO2 simultaneously. Here, we report an alternative approach to address this challenge by developing a new melt-solid interface through the in situ alkali metal surface segregation and consecutive eutectic formation at perovskite oxide surface at PCFC operating temperatures. This new approach in cathode engineering is successfully demonstrated over a lithium and sodium co-doped BaCo0.4Fe0.4Zr0.1Y0.1O3-δ perovskite as the model material. Our experimental results unveil that the unique in situ formed melt-solid surface stabilises the catalytically active phase in the bulk and promotes catalytically active site at surface. Our novel engineered melt-solid interface enhanced the stability of the cathode against poisoning in 10% CO2 by a factor of 1.5 in a symmetrical cell configuration and by a factor of more than two in PCFC single cells.

Modulating the liquid phase of metal-organic frameworks (MOFs) presents new opportunities for functionalizing glassy MOFs, expanding the fundamental science and practical application for this emerging family of materials. Herein, we report the fabrication of a bimetallic glassy MOF via a liquid-liquid transition process. This is achieved by introducing a robust Schiff base-cobalt functional group into Zn-ZIF-62, which attracts negatively charged imidazolate ligands, facilitating low-temperature melting. This ultimately leads to the formation of a bimetallic glassy MOF (Co/Zn-agZIF-62-ipy) upon melt-quenching. The material features an exceptionally high glass-forming capability, uniformly distributed bimetallic ions, and a markedly enhanced visible light photogeneration efficiency of enzymatically active nicotinamide adenine dinucleotide (NADH) when compared with Co-doped ZIF-62 glass. These findings offer novel insights into modulating the liquid phase of an MOF to develop functional glassy MOF photocatalysts for coenzyme NADH regeneration and other advanced applications.

Traditional oil/water emulsion separation membranes often fail to maintain long-term stability and regeneration due to inadequate fouling resistance and low self-cleaning efficiency in practical applications. This study developed a superhydrophilic nanofiber membrane with a micro/nanolayer architecture and piezoelectric photocatalytic properties by combining polyacrylonitrile (PAN), polyethyleneimine (PEI), and silver-modified barium titanate (Ag-DBT). This membrane can effectively separate oils and dyes from complex emulsions, demonstrating high water permeation flux of 2492 L.m(-2).h(-1), along with exceptional oil separation efficiency (similar to 99 %) and dye adsorption (similar to 99 %). In addition, the PAN-PEI/Ag-DBT membrane demonstrated an ultra-high degradation efficiency of approximately 99 % for methyl blue (MB) within 90 min. Notably, owing to the piezoelectric photocatalytic properties of Ag-DBT, the PAN-PEI/Ag-DBT nanofiber membrane maintained exceptional self-cleaning performance even after high contamination. To assess the self-cleaning performance and cycling stability of the PAN-PEI/Ag-DBT membrane, we conducted cyclic recovery experiments across three conditions: oil-in-water emulsions, dye-water solutions, and oil-in-dye-water emulsions. In the first three self-cleaning cycles, the self-cleaning membrane demonstrated water flux recovery rates that exceeded 90 % and irreversible fouling rates that were below 10 %. This research provides new insights into the advancement of multifunctional self-cleaning membranes.

Efficient and reliable protonic ceramic fuel cells (PCFCs) necessitate the development of active and durable cathode materials to accelerate the sluggish oxygen reduction reaction (ORR). The most promising PCFC cathode candidates are perovskite‐type structured oxides with mixed oxygen ion, proton, and hole conductivity. However, mixed conductivity often requires materials with alkaline earth elements and the inclusion of these elements in the cathode structure leads to severe degradation in the presence of even small trace amounts of CO 2 in air. Herein, a new approach is presented to address this challenge by inducing selective in situ phase segregation to engineer the cathode surface and bulk separately. This selective phase segregation is achieved via targeted control of the size mismatch of cations in the perovskite‐type structure, enhancing charge transfer in the bulk while improving CO 2 resistance at the surface. By co‐incorporating smaller Li + and larger K + into the model BaCo 0.4 Fe 0.4 Zr 0.1 Y 0.1 O 3−δ cathode material, it is shown that Li + segregates to the surface, protecting it from CO 2 poisoning, while K + remains in the bulk and accelerates proton transport. Consequently, this in situ restructured cathode can boost the PCFC power output by 30% and improve its CO 2 tolerance fivefold in the presence of CO 2 at 600 °C.

Membrane-based gas separation technologies have attracted significant attention for their energy efficiency and environmental benefits. As a type of promising candidate material, MOF glass has shown great potential in the gas separation membrane by improving interfacial compatibility with other functional components and processability toward continuous, pinhole-free films. In this study, we report the development of self-supporting MOF crystal-glass composite membranes by integrating UiO-66 crystals into a melt-processable zinc coordination polymer glass (agZnCP_bim, where ag represents amorphization by glass formation) matrix. The ZnCP_bim exhibited a low melting temperature and a high glass-forming ability, allowing for in situ melt-quenching to form defect-minimized MOF crystal-glass composite membranes. UiO-66/agZnCP_bim composite membranes with varying UiO-66 loadings (up to 50 wt %) were fabricated to investigate the effect of the filler content on membrane properties. Structural characterizations confirmed the preservation of the UiO-66 crystallinity and the amorphous nature of the ZnCP_bim glass matrix. In situ THz-FarIR spectroscopy revealed strong interfacial interactions and irreversible structural transitions during thermal processing. Gas adsorption-desorption of CO2 and N2 showed the increased porosity introduced by UiO-66 and enhanced affinity for CO2 molecules. Gas permeation measurements of self-supporting UiO-66/agZnCP_bim membranes for N2/CH4 and H2/CO2 showed a notable improvement in both permeability and selectivity, which exceeded the Robeson upper bound.

Due to their unique properties, noble gases are significant in various disciplines despite their relative scarcity in the Earth's atmosphere. However, capturing and purifying noble gases from gas mixtures remains...

The persistence of defects in polycrystalline membranes poses a substantial obstacle to reaching the theoretical molecular sieving separation and scaling up production. The low membrane selectivity in most reported literature is largely due to the unavoidable non-selective defects during synthesis, leading to a mismatch between the well-defined pore structure of polycrystalline molecular sieve materials. This paper presents a novel approach for minimizing non-selective defects in metal–organic framework (MOF) membranes by a constricted crystal growth strategy in a confined environment. The in situ ZIF formation using the densely packed seeding array between the substrate and the pre-grown top ZIF layer yields a confined membrane interlayer, which is highly uniform with a tightly packed crystalline structure. Unlike uncontrolled crystal growth, we purposely regulate the interlayer membrane growth in the direction parallel to the substrate. A notable 99 % decrease in defects in the confined interlayer was achieved compared to the random-grown top layer, leading to a ~353 % increment in H 2 /N 2 selectivity over the non-confined reference MOF membrane. The performance of this new membrane sits in the optimal range above the Robeson upper bound. The membrane boasts a balanced high H 2 permeability (>5000 Barrer) and selectivity (>50), significantly surpassing peer ZIF membranes.

UiO-66-NH2 ([Zr6O4(OH)4(NH2-bdc)], NH2-bdc = 2-aminoterephthalic acid) was post-synthetically modified using four strategies to improve its external hydrophobicity. The modified MOFs exhibited increased hydrophobicity to water droplets, but their internal hydrophobicity remained unchanged. This highlights a disconnect between hydrophobicity towards vapour and liquid water, referred to as the Gore-Tex (R) effect. UiO-66-NH2 ([Zr6O4(OH)4(NH2-bdc)], NH2-bdc = 2-aminoterephthalic acid) was post-synthetically modified using four strategies to improve its external hydrophobicity.

Metal–organic framework (MOF) glass is a versatile and processible material that retains its porous nature while transitioning between liquid and solid states. Incorporating composites into MOF glass can enhance its functionalities, but the effect of the added material on the solid–liquid phase transition of MOF glass remains understudied. This research explores the impact of silver ions on the properties of ZIF‐62 glass, revealing their influence on phase conversion at varying ligand concentrations. The presence of silver enhances gas separation processes, particularly improving CO 2 and hydrocarbon separation selectivity compared to pure ZIF‐62 glass. These findings provide valuable insights for composite integration and highlight the potential of AgZIF‐62 glass in gas separation applications. Furthermore, this work paves the way for processing functional AgZIF‐62 glass films, enabling diverse applications such as gas separation, film catalysis, and antimicrobial glass.

Impregnated zeolite-carbon (IZC), also known as pore-modified zeolite, was used as a potential filler in a P84 co-polyimide-based hollow fiber mixed matrix membrane (HF MMM) to enhance gas separation. The presence of carbon structure on the zeolite framework pore was to avoid the trapped moisture that could lead to permeability reduction. This work seeks to investigate the impact of IZC addition (0.5, 1.0, and 1.5wt%) to the P84 membrane and examine its permeability and separation performance. Adding IZC filler to the P84 membrane generates the enhancement of gas selectivity and permeability. The optimal enhancement was observed at 1wt% of IZC loading, in which selectivity of CO2/CH4, CO2/N2, O2/N2, H2/N2, and H2/CH4 was enhanced by 50.506, 51.042, 5.693, 16.712, and 16.338%, respectively. On the other hand, H2, CO2, and O2 permeability at the loading were improved from 11.182 to 26.761, from 4.683 to 14.501, and from 1.637 to 3.546 Barrer, respectively. The improvement of gas selectivity was contributed by the presence of carbon in the zeolite framework, providing a molecular sieving effect while tuning carbon properties with pore regularity by templating in the zeolite framework enhances the gas permeability.