Conventional rechargeable zinc-air batteries (ZABs) face two critical challenges: (1) slow kinetics of the oxygen reduction (ORR) and oxygen evolution (OER) reactions; and (2) the thermodynamic incompatibility of OER and ORR occurring concurrently on a single air cathode. To address these limitations, we propose in this study a dual-cathode zinc-ethylene glycol/air battery (D-ZEAB) that spatially decouples ORR and the ethylene glycol oxidation reaction (EGOR) onto separate cathodes, enabling concurrent electricity generation and electroreforming of polyethylene terephthalate (PET) plastic waste into high-value C2 chemicals. Furthermore, we develop a bifunctional catalyst composed of defect-rich subnanometer-thick PdCuCo trimetallenes to enhance both EGOR and ORR kinetics. Benefiting from the decoupled cathode configuration and the bifunctional PdCuCo catalyst, the D-ZEAB demonstrates an energy conversion efficiency of 91.7%, a long cycle life of 1696 h, and a Faradaic efficiency of >93% for GA production. This work not only presents a promising strategy for advancing the zinc-air battery technology but also offers a sustainable route for simultaneous energy storage and plastic waste upcycling.

ABSTRACT Many of the membraneless organelles inside cells are multiphasic condensates with complex structural organizations driven by the demixing of phase‐separating proteins. Tailoring the structures of multiphasic condensates by controlling their demixing states is a challenge. Here, we employ two proteins with distinctly different features, including thermal responsiveness, hydrophobicity, and charges: a positively charged RGGRGG protein, which forms phase‐separated condensates below an upper critical solution temperature, and a protein based on an elastin‐like polypeptide, which forms condensates above a lower critical solution temperature. These two proteins demix to form multiphasic condensates with nested and core‐shell structures under variable conditions, which can be tailored by altering the physical and chemical environments. The demixed multiphasic condensates can also be constructed inside Escherichia coli cells, recapitulating the properties of membraneless organelles. We also show that nucleic acids preferentially enrich in the positively charged segment of the multiphasic condensates. Lastly, multiphasic condensates can deliver nucleic acids across the plasma membrane into mammalian cells, enabling cell transfection.

Excessive fluoride (F-) in water environment seriously endangers ecological security. This study constructed a series of dual-metal loaded biochar adsorbents (CeFe@BC) by modifying cerium-based materials through Fe doping and coupling with straw-derived biochar substrates. Ce9Fe1@BC11 exhibited a remarkable F- adsorption capacity of 110.32 mg/g and had broad operational pH range (q(e(pH=2)(-)(12)) >= 82.61 mg/g). It showed exceptional selectivity and affinity toward F- even in multicomponent systems. The adsorption process was successfully characterized by pseudo-second-order kinetic (R-2 >= 0.999) and Temkin isotherm model (R-2 >= 0.952), indicating a chemisorption-dominated mechanism. Mechanistic studies revealed that Fe(II) doping maintained the quantity of Ce(III) active adsorption sites through the Fe(II)/Ce(IV) redox reactions, enabling the inverse transformation from Ce(IV) to Ce(III), rather than participating directly in adsorption. This regeneration mechanism increased the number of adsorption active sites of the material by re-reducing Ce(IV) back to Ce(III) during fluoride adsorption or desorption, thereby significantly enhancing adsorption performance. Unlike other anions that adsorb solely via substitution of terminal hydroxyl groups (T-OH) on metal oxides, fluoride onto CeFe@BC exhibited a dual-site adsorption behavior, involving both T-OH substitution and occupancy of bridging hydroxyl (B-OH) sites. Consequently, the T-OH and B-OH groups coordinated with Ce(III) constitute the primary active adsorption sites. The hierarchical porous structure of the straw biochar exposed abundant adsorption sites and also enhanced electron transfer during redox cycles due to its superior conductivity, enabling regeneration of Ce(III) active sites. This work provided a novel strategy for the synergistic structural-functional modulation of high-performance fluoride adsorbents, advancing the rational design of materials for environmental remediation.

Herein, nickel foam supported NiFeCoCr medium-entropy Hoffmann-type coordination polymer (NiFeCoCr-HCP/NF) nanosheet arrays comprising Ni2+, Co2+, Fe3+, Cr3+, and a potassium tetracyano nickelate ligand were fabricated for the first time. NiFeCoCr-HCP/NF demonstrated superior UOR performance with a low potential of 1.45 V (vs. RHE) at 100 mA cm-2 and strong operational stability, highlighting Ni-based HCP materials as efficient, economical electrocatalysts.

The oxygen evolution reaction (OER) in conventional zinc-air batteries (ZABs) involves a complex multielectron transfer process, leading to slow reaction kinetics, high charging voltage, and low energy efficiency. To address these limitations, a zinc-ethanol/air battery (ZEAB) system that strategically replaces the OER with the ethanol oxidation reaction (EOR) possessing a lower thermodynamic potential has been proposed. Herein, a bimetallic catalyst CuCo-embedded nitrogen-doped carbon (CuCo-20%-1), derived from a Cu/Co/Cd co-coordinated metal-organic precursor, is synthesized and exhibits an excellent performance for both EOR and ORR. A series of characterizations and in situ Raman spectroscopy analyses confirmed the formation of high-density M-Nx sites and Cu-doped CoOOH through an in situ electrochemical process from bimetallic CuCo species as the catalytic active sites for the oxygen reduction reaction (ORR) and EOR, respectively. Combined density functional theory calculations elucidated the catalytic reaction pathway and enhancement mechanism of Cu doping in CoOOH for EOR. The ZEAB system exhibits remarkable operational metrics, achieving an energy efficiency of 63.4%, representing a 32.7% energy consumption reduction compared to conventional ZABs. This strategic alternative model from the OER to EOR not only circumvents the fundamental kinetic limitations but also establishes a possible framework for promoting the practical application of next-generation metal-air battery technology.

Fluoride (F-) pollution in surface water seriously endangers ecological safety. Cerium-based adsorbents have original advantages in adsorbing F- such as abundant oxygen vacancies and variable valence states. However, high cost and separation difficulty limit their application in fluoridated surface water treatment. This work synthesized bimetallic oxide adsorbents (FeCe@C) to enhance the efficacy of cerium-based adsorbents for F- removal and systematically examined how Fe(II) doping influenced fluoride removal efficiency. Results indicated that FeCe@C adsorbed F- better than the pure Ce-based adsorbent (Ce@C), with q(max) = 243.31 mg/g at 25 degrees C, and reached adsorption equilibrium in merely five minutes, with significantly better adsorption performance than fluoride adsorbents reported in previous literature. F- adsorption process aligned with the Temkin (R-2 > 0.963), pseudo-second-order kinetic (R-2 > 0.999) and Elovich model (R-2 > 0.993), suggesting that the F- adsorption mechanism was governed by chemisorption-dominated heterogeneous surface reactions. Further results proved that the doping of iron exhibited a significant effect on the generation of Ce(III) active sites and oxygen vacancies in FeCe@C, which showed a positive correlation (R-2 = 0.87 and 0.98). And unlike other metal doping mechanisms, the doped Fe species promoted the formation of Ce(III) through redox reactions during the adsorption process, achieving the reverse conversion of Ce(IV) to Ce(III), rather than directly participating in adsorption. Density functional theory (DFT) calculations demonstrated that iron doping effectively enhanced electron transfer and the interaction between F- and the adsorbent, resulting in a higher F- adsorption capacity. This study provides fundamental theory for enhanced fluoride removal and offers new ideas for elevating the efficacy of cerium-based adsorbents.

The alumina industry faces critical sustainability challenges from massive red mud (RM) discharge, which occupies vast land areas and poses severe environmental risks. Moreover, inefficient iron recovery from RM, due to poor mineral liberation, leads to the loss of valuable iron resources. This study introduces triethanolamine (TEOA) as a sustainable alternative to lime in the Bayer digestion to address these challenges. Optimal digestion conditions (265 degrees C, 10 wt % TEOA/bauxite, 100 min, 230 g/L Na2O), identified via full factorial design, achieved an iron recovery rate of 89.04% from RM via magnetic separation. The resulting iron concentrate (60.26% Fe) is an excellent secondary iron resource. Crucially, this integrated approach led to an 84.10% reduction in RM discharge as compared to the conventional lime-based method. The mechanism of TEOA-enhanced Bayer digestion was investigated through thermodynamic and kinetic studies, complemented by DFT calculations. TEOA decomposition was found to generate atomic hydrogen (H center dot), which reduces FeO2 - on hematite surfaces to HFeO2 -, promoting the transformation of hematite into magnetite. Concurrently, HFeO2 - reacts with anatase to form ilmenite, which inhibits sodium titanate formation, thus ensuring high aluminum extraction efficiency with 95.97%. This work presents a novel and sustainable strategy for significantly reducing RM discharge and enhancing iron valorization in the alumina industry, offering a pathway toward a more circular economy.

This study first evaluated the sulfamethoxazole (SMX) effects on oxygen-reducing biocathodes in microbial fuel cells (MFCs). Low SMX (0.5 mg L-1) enhanced current density by 20 % via increased direct electron transfer and lower charge transfer resistance. High SMX (10-30 mg L-1) suppressed electrochemical performance. SMX preferentially bound protein-like EPS components over fulvic-like fractions, inducing sequential structural changes (1054 > 970 > 3464 > 2921 > 1643 > 1350 cm-1). SMX exposure reshaped microbial communities, enriching antibiotic-resistant genera (Truepera, Nitrospira, Brevundimonas, etc.). Network analysis revealed low SMX enhanced community complexity/stability, while high doses simplified biofilm structure. Functional genes for electron transfer, carbon metabolism and oxidative phosphorylation increased at 0.5 mg L-1 SMX but decreased under high concentrations. Overall, this study elucidates the dual role of SMX in modulating oxygen-reducing biofilm composition, function, and capability, laying the groundwork for optimized application of MFC in treating SMX-contaminated wastewater.

BACKGROUND:Fungal phytopathogens pose a significant threat to global crop yields. The overuse of pesticides leads to pesticide-resistant pathogens, environmental contamination and risks to human health. Consequently, there is an urgent need for effective and ecofriendly antifungal strategies to address these challenges. RESULTS:Herein, ZnO-ZIF-8 is synthesized via an in situ growth method to integrate the antifungal property of zinc oxide (ZnO) and the control release property of zeolitic imidazolate framework (ZIF)-8. Results suggest that the inhibition rates of ZnO, ZIF-8 and ZnO-ZIF-8 against Alternaria alternata are 44.4%, 74.1% and 94.4%, respectively, indicating that ZnO-ZIF-8 exhibits the most potent antifungal activity. ZnO-ZIF-8 also causes distortion and fracture of mycelia, significantly impairing spore germination and inhibiting germ tube elongation. CONCLUSION:The potential antifungal mechanisms of ZnO-ZIF-8 involve the disruption of fungal cell morphology and structure through the release of Zn2+, ultimately leading to fungal cell death. Biosafety assessments indicate that the application of ZnO-ZIF-8 exhibits negligible effects on tobacco seeds and plants. This study provides valuable insights for the effective management of plant fungal diseases and supports sustainable agricultural development. © 2025 Society of Chemical Industry.

The composite photocatalyst FeOOH/g-C3N4 was prepared through thermal polycondensation and co-precipitation methods, followed by XRD, SEM and UV-vis characterization. The stability of FeOOH/g-C3N4 was explored by the recycling test. The active species in the reaction system were investigated by the capture experiment. The results indicated that the optimal preparation condition for g-C3N4 involved calcination at 600 °C for 4 h. XRD analysis revealed that g-C3N4 exhibits a high-purity phase, and Fe in FeOOH/g-C3N4 exists in a highly dispersed amorphous state. SEM analysis showed that FeOOH/g-C3N4 has a rough surface with an irregular layered structure. Element composition analysis confirmed that the content of elements in the prepared catalyst is consistent with the theoretical calculation. FeOOH/g-C3N4 possesses the largest specific surface area of 143.2 m2/g and a suitable pore distribution. UV-vis DRS analysis showed that the absorption intensity of FeOOH/g-C3N4 is stronger than that of g-C3N4. When the catalyst dosage was 1.0 g/L, the H2O2 dosage was 4 mmol/L, the PNP initial concentration was 10 mg/L and the initial pH value was 5, the PNP removal could reach 92% in 120 min. Even after 5 cycles, the efficiency of PNP removal by FeOOH/g-C3N4 remains nearly 80%. The capture experiment indicated that both •OH and •O2− play roles in the photocatalytic degradation of PNP, with •OH being more significant. These findings affirm that FeOOH has been successfully incorporated into g-C3N4, resulting in a conspicuous catalytic effect on the degradation of PNP in the visible light-assisted Fenton-like reaction.

Urea electrolysis is considered as a promising energy-saving hydrogen production technique to substitute the water electrolysis, but it is restricted by the lack of efficient and cost-effective catalysts. Herein, nickel foam supported three-dimensional (3D) nickel-organic framework nanosheet arrays (Ni-BDC-t/NF, where t is the reaction time) comprising Ni2+ and an organic ligand of 4,4-biphenyl dicarboxylic acid (BDC) are synthesized as catalyst for urea electrolysis in alkaline media. Benefiting from the highly exposed Ni active sites and fast electron transfer rate endowed by 3D nanosheet array architecture, the structurally optimized Ni-BDC-10/NF exhibits preeminent electrocatalytic activity and durability toward urea oxidation reaction (UOR). To deliver a high current density of 100 mA cm-2, the required UOR potential of Ni-BDC-10/NF is only 1.50 V vs. RHE. Significantly, by further coupling with the cathodic hydrogen evolution reaction, the urea electrolysis system based on Ni-BDC-10/NF self-supporting anode exhibits a dramatic voltage decrease by 340 mV at a current density of 50 mA cm-2 as compared with that of water electrolysis under the same conditions. This study provides some new ideas for developing high-efficiency nickel-based organic framework catalysts and their application in urea-related energy storage devices.

Developing highly efficient electrocatalysts for organic electrosynthesis such as the nucleophile oxidation reaction (NOR) is of great significance for renewable energy utilization. However, the kinetic understanding of nickel-based catalysts in NOR still needs to be clarified. Herein, we synthesized several metal ions-doped Ni(OH)(2) and studied the mechanism of metal ions doping in enhancing the electrocatalytic NOR performance. Ethanol oxidation reaction (EOR) was used as a model reaction and a series of electrochemical measurements for the reaction order, electron transfer process, and metal redox kinetics of Ni(II)/Ni(III) were combined with the electronic structural characterization and theoretical calculation. The rate-determining step (RDS) of EOR was confirmed as the oxidation process of Ni(II)-OH to Ni(III)-O with one electron transfer; meanwhile, the kinetic mechanism of metal ions doping was unveiled: (1) decreasing the oxidation potential of Ni(II)-OH to Ni(III)-O was achieved by enhancing the interaction between the adjacent Ni and O and lowering the O-H bond dissociation energy barrier; (2) accelerating the cycling kinetics of Ni(II)/Ni(III) redox by bimetallic synergy improved the electronic transfer ability of materials. Our study is valuable in deeply understanding the kinetic mechanism of the synergetic electrochemical-chemically involved reaction processes in NOR.

Transition metals, which are of diversity in their bonding orbitals, have a variety of significant oxidation states , more complex chemical properties compared to the main group metals. Of particular importance, devel-opment of transition metals-mediated catalysis with high activity and stability is a challenging and prospective research hotspot. On the other hand, since the high dependence on petroleum-based raw materials has shown an indelible impact on the environment, it is imminent for the entire society to develop green, renewable , sustainable energy to achieve the vital goal of reducing carbon emissions. Renewable biomass, the most suitable alternative of organic carbon sources to replace fossil resources, is believed to produce chemicals that can include almost all fossil-based products. The consolidation of biomass and its derived molecules into industrial pro-duction can, in principle, enable the sustainable synthesis of high-value-added products such as organonitrogen compounds of N-heterocycles having extensive applications. Importantly, transition metals have partially filled or empty d orbitals, which confer them a distinct catalytic selectivity and superior stability over the main group metals in terms of catalysts preparation like metal-organic frameworks (MOFs), organometallic complexes, and single atoms, especially for sustainable construction of N-heterocycles from biomass feedstocks. This review focuses on the research progress on transition metals catalysis for promoting the selective synthesis of various classes of N-heterocycles by using biomass and its derivatives as substrates or intermediates. The development of transition metals-based heterogeneous and homogeneous catalytic systems and their advantages are highlighted through typical C-N bond-forming coupling reactions. Moreover, the synthesis of N-heterocycles mediated by transition metals-based catalysts is discussed in detail from the perspectives of catalytic modes (thermocatalysis, photocatalysis, and electrocatalysis), catalyst design strategies, structure-activity relationships, and crucial re-action mechanisms. Finally, the current challenges and prospects in N-heterocycles synthesis from biomass feedstocks by transition metals-catalyzed manner are presented to provide interesting guidance for future research, such as precise designing of transition metals-based catalysts and benign broadening of product range of renewable N-heterocycles. This review hopes to provide updated knowledge and perspectives, serving as an important resource to inspire novel ideas and approaches in the field of catalysts design that will facilitate the advancement of sustainable synthesis.

Water pollution has become one of the most important global environmental pollution problems, wherein various toxic and persistent organic pollutants in water pose a major threat to the environment. Significantly, photocatalysis is considered an efficient technique, demonstrating great advantages for the removal of organic pollutants for wastewater treatment. Lately, metal-organic frameworks (MOFs), which are a group of organic-inorganic hybrid materials possessing an outstanding pore structure, adsorption capacity, and photocatalytic property, have demonstrated great promise as effective photocatalysts. Significant progress has been achieved in the application of MOFs for the degradation of organic pollutants, and thus they have attracted widespread attention from the research community and industry. This review aims to summarize the recent advances in the preparation and strategies for the modification of MOF-based photocatalysts, as well as the progress in their state-of-the-art application in the degradation of organic pollutants. Some heterojunctions formed by MOF-based composite photocatalysts are expounded in detailed. More importantly, the corresponding working mechanisms for the photocatalytic degradation of pesticides, antibiotics, and dyes driven by MOF-based photocatalysts are demonstrated. Further, a series of key parameters affecting the photocatalytic degradation process is briefly analyzed. Finally, the outlooks and challenges of MOF materials for the removal of organic pollutants in water are emphasized. It is hoped that this review will provide some meaningful inspiration and references for the future development of MOF-based photocatalysts with greater photocatalytic performance for wastewater treatment.

Abstract Thermochemical conversion of fossil resources into fuels, chemicals, and materials has rapidly increased atmospheric CO2 levels, hindering global efforts toward achieving carbon neutrality. With the increasing push for sustainability, utilizing electrochemical technology to transform CO2 or biomass into value‐added chemicals and to close the carbon cycle with sustainable energy sources represents a promising strategy. Expanding the scope of electrosynthesis technology is a prerequisite for the electrification of chemical manufacturing. To this end, constructing the C─N bond is considered a priority. However, a systematic review of electrocatalytic processes toward building C─N bonds using CO2 and biomass as carbon sources is not available. Accordingly, this review highlights the research progress in the electrosynthesis of organic nitrogen compounds from CO2 and biomass by C─N coupling reactions in view of catalytic materials, focusing on the enlightenment of traditional catalysis on C─N coupling and the understanding of the basis of electrochemical C─N coupling. The possibility of C─N bond in electrocatalysis is also examined from the standpoints of activation of substrates, coupling site, mechanism, and inhibition of hydrogen evolution reaction (HER). Finally, the challenges and prospects of electrocatalytic C─N coupling reactions with improved efficiency and selectivity for future development are discussed.

In nature, enzymes that catalyze sequential reactions are often assembled as clusters or complexes. The formation of multienzyme complexes, or metabolons, brings the enzyme active sites into proximity to promote intermediate transfer, decrease intermediate leakage, and streamline the metabolic flux towards the desired products. We and others have developed synthetic versions of metabolons through various strategies to enhance the catalytic rates for synthesizing valuable chemicals inside microbes. Synthetic multienzyme complexes range from static enzyme nanostructures to dynamic enzyme coacervates. Enzyme complexation optimizes the metabolic fluxes inside microbes, increases the product titer, and supplies the field with high‐yield microbe strains that are amenable to large‐scale fermentation. Enzyme complexes constructed inside microbial cells can be separated as independent entities and catalyze biosynthetic reactions ex vivo; such a feature gains these complexes another name, “synthetic organelles” – new subcellular entities with independent structures and functions. Still, the field is seeking new strategies to better balance dynamicity and confinement and to achieve finer control of local compartmentalization in the cells, as the natural multienzyme complexes do. Industrial applications of synthetic multienzyme complexes for the large‐scale production of valuable chemicals are yet to be realized. This review focuses on synthetic multienzyme complexes that are constructed and function inside microbial cells.

The disadvantages of layered double hydroxides (LDHs) such as easy stacking, poor inherent conductivity, and limited versatility hinder their application in splitting water and zinc-air batteries (ZABs). Interface engineering to regulate the electron distribution of LDHs by introducing another component is a way to compensate for the poor electron transport capacity of LDHs during catalysis. Herein, a hierarchical structure is synthesized by assembling CoFe-LDH nanosheets onto the surface of layered N-doped porous carbon (NPC), CoFe-LDH@NPC, by using an interface engineering strategy. CoFe-LDH@NPC has high catalytic activity for the oxygen/hydrogen evolution reaction (OER/HER) with overpotentials of 280/100 mV, respectively. The two-electrode water splitting catalyzed by CoFe-LDH@NPC only needs 1.61 V to drive a current density of 10 mA cm-2 for 60 h. The theoretical results show that there is an electron-deficient/electron-rich interface between the NPC substrate and the CoFe-LDH in CoFe-LDH@NPC. The electrons on the coupling interface are easily transferred, which results in a change of the adsorption behavior of the reaction intermediates and improves the catalytic activity for the OER and HER. In addition, CoFe-LDH@NPC-catalyzed rechargeable flexible ZABs have excellent performance with low charge-discharge polarization (0.87 V) and a long-term stability of 65 h.

Iron coordinated with nitrogen (FeNx) sites hosted in the micropores of carbon substrate offer excellent performance for the oxygen reduction reaction (ORR). Achieving a highly exposed and dispersed FeNx sites accessible for ORR is still challenging to date. In this work, two-dimensional hexagonal carbon nanosheets supported FeNx moieties (FeNC-NaCl-T) were synthesized via a molten NaCl-assisted pyrolysis strategy. Benefit from the high specific surface area (1371.635 m3 center dot g-1) and highly dispersed FeNx sites, the optimized FeNC-NaCl-900 exhibits superior ORR activity with a high half-wave potential of 0.90 V in alkaline electrolyte. Impressively, with FeNC-NaCl-900 as the cathode catalyst in aqueous zinc-air battery, achieving a remarkable performance with a high peak power density of 177 mW center dot cm-2 and competitive durability (200 h). Furthermore, the Al-air battery equipped with FeNC-NaCl-900 attained an ultrahigh specific capacity of 2257.48 mAh center dot g-1 ata large discharge current of 100 mA cm-2. These findings provide guidance for the development of high performance FeNC catalysts and their applications in metal-air batteries.

One-pot green urea electrosynthesis from CO2 and nitrogenous pollutants via the co-reductive C - N coupling route under ambient conditions is prospective to replace the traditional urea synthesis process. Here, a bifunctional indium hydroxide (Vo-S-IO-6) bearing oxygen vacancy (Vo) sites on {100} facets was developed to markedly enable urea synthesis (unprecedented faradaic efficiency of 60.6% with a high production rate of 910.4 mu g h(-1) mg(cat)(-1).) from NO3- and CO2 by subtly integrating facet and defect engineering. ln-O-x-O-ln (x = C or N) configuration and Vo in Vo-S-IO-6 provided dual active sites for the adsorption and activation of NO3- and CO2 to exclusively form *NO2 and *CO2 species, respectively, which ensured highly selective C N coupling. Moreover, theoretical calculations elaborated that Vo-induced local electron reconstruction accelerated the protonation rate-determining step, thus lowering overall energy barriers. This work offers a design strategy of synergistic electrocatalysts based on geometrical nature for efficient urea synthesis.