Matrix-Free Thermally Activated Delayed Fluorescent Carbon Dots-Based Electroluminescent Light-Emitting Diodes Exceeding 5.6% External Quantum Efficiency.

Carbon dots (CDs) are promising luminescent emission layer materials for next generation electroluminescent light emitting diodes (EL-LEDs) due to their many advantages, such as environmental friendliness, low cost, and high stability. However, limited by the spin-forbidden properties of the triplet transition, it is difficult to improve the external quantum efficiency (EQE) of fluorescent CDs-based EL-LEDs. Meanwhile, traditional thermally activated delayed fluorescent (TADF) CDs prepared using coating strategies are difficult to utilize in EL-LEDs due to the nonconductivity of the coating agent. Herein, we successfully developed matrix-free TADF CDs with yellow emission and achieved a device EQE of 5.68%, which is the highest value reported in CDs-based EL-LEDs. In addition, we also developed white EL-LEDs with an EQE of 1.70%. This study highlights the importance of interactions between precursors in modulating the electroluminescence properties of TADF emitters and provides an effective design principle for matrix-free TADF CDs.

Pore Space Partition Synthetic Strategy in Imine-linked Multivariate Covalent Organic Frameworks.

Partitioning the pores of covalent organic frameworks (COFs) is an attractive strategy for introducing microporosity and achieving new functionality, but it is technically challenging to achieve. Herein, we report a simple strategy for partitioning the micropores/mesopores of multivariate COFs. Our approach relies on the predesign and synthesis of multicomponent COFs through imine condensation reactions with aldehyde groups anchored in the COF pores, followed by inserting additional symmetric building blocks (with C2 or C3 symmetries) as pore partition agents. This approach allowed tetragonal or hexagonal pores to be partitioned into two or three smaller micropores, respectively. The synthesized library of pore-partitioned COFs was then applied for the capture of iodine pollutants (i.e., I2 and CH3I). This rich inventory allowed deep exploration of the relationships between the COF adsorbent composition, pore architecture, and adsorption capacity for I2 and CH3I capture under wide-ranging conditions. Notably, one of our developed pore-partitioned COFs (COF 3-2P) exhibited greatly enhanced dynamic I2 and CH3I adsorption performances compared to its parent COF (COF 3) in breakthrough tests, setting a new benchmark for COF-based adsorbents. Results present an effective design strategy toward functional COFs with tunable pore environments, functions, and properties.

Oxygen Radical Coupling on Short-Range Ordered Ru Atom Arrays Enables Exceptional Activity and Stability for Acidic Water Oxidation.

The discovery of efficient and stable electrocatalysts for oxygen evolution reaction (OER) in acid is vital for the commercialization of the proton-exchange membrane water electrolyzer. In this work, we demonstrate that short-range Ru atom arrays with near-ideal Ru-Ru interatomic distances and a unique Ru-O hybridization state can trigger direct O*-O* radical coupling to form an intermediate O*-O*-Ru configuration during acidic OER without generating OOH* species. Further, the Ru atom arrays suppress the participation of lattice oxygen in the OER and the dissolution of active Ru. Benefiting from these advantages, the as-designed Ru array-Co3O4 electrocatalyst breaks the activity/stability trade-off that plagues RuO2-based electrocatalysts, delivering an excellent OER overpotential of only 160 mV at 10 mA cm-2 in 0.5 M H2SO4 and outstanding durability during 1500 h operation, representing one of the best acid-stable OER electrocatalysts reported to date. 18O-labeled operando spectroscopic measurements together with theoretical investigations revealed that the short-range Ru atom arrays switched on an oxide path mechanism (OPM) during the OER. Our work not only guides the design of improved acidic OER catalysts but also encourages the pursuit of short-range metal atom array-based electrocatalysts for other electrocatalytic reactions.

Deeper Insights into the Morphology Effect of Na2Ti3O7 Nanoarrays on Sodium-Ion Storage.

Na2Ti3O7-based anodes show great promise for Na+ storage in sodium-ion batteries (SIBs), though the effect of Na2Ti3O7 morphology on battery performance remains poorly understood. Herein, hydrothermal syntheses is used to prepare free-standing Na2Ti3O7 nanosheets or Na2Ti3O7 nanotubes on Ti foil substrates, with the structural and electrochemical properties of the resulting electrodes explored in detail. Results show that the Na2Ti3O7 nanosheet electrode (NTO NSs) delivered superior performance in terms of reversible capacity, rate capability, and especially long-term durability in SIBs compared to its nanotube counterpart (NTO NTs). Electrochemical impedance spectroscopy (EIS) and scanning electron microscopy (SEM) investigations, combined with density functional theory calculations, demonstrated that the flexible 2D Na2Ti3O7 nanosheets are mechanically more robust than the rigid Na2Ti3O7 nanotube arrays during prolonged battery cycling, explaining the superior durability of the NTO NSs electrode. This work prompts the use of anodes based on Na2Ti3O7 nanosheets in the future development of high-performance SIBs.

Synergistic Interfacial Effect of Ru/Co3O4 Heterojunctions for Boosting Overall Water Splitting.

Low-cost bifunctional electrocatalysts capable of efficiently driving the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are needed for the growth of a green hydrogen economy. Herein, a Ru/Co3O4 heterojunction catalyst rich in oxygen vacancies (VO) and supported on carbon cloth (RCO-VO@CC) is prepared via a solid phase reaction (SPR) strategy. A RuO2/Co9S8@CC precursor (ROC@CC) is first prepared by loading Co9S8 nanosheets onto CC, following the addition of RuO2 nanoparticles (NPs). After the SPR process in an Ar atmosphere, Ru/Co3O4 heterojunctions with abundant VO are formed on the CC. The compositionally optimized RCO-VO@CC electrocatalyst with a Ru content of 0.55 wt.% exhibits very low overpotential values of 11 and 253 mV at 10 mA cm-2 for HER and OER, respectively, in 1 m KOH. Further, a low cell voltage of only 1.49 V is required to achieve a current density of 10 mA cm-2. Density functional theoretical calculations verify that the outstanding bifunctional electrocatalytic performance originates from synergistic charge transfer between Ru metal and VO-rich Co3O4. This work reports a novel approach toward a high-efficiency HER/OER electrocatalyst for energy storage and conversion.

Insightful Understanding of Synergistic Oxygen Reduction on PtCo3(111) Toward Zinc-Air Batteries.

Theory-guided materials design is an effective strategy for designing catalysts with high intrinsic activity whilst minimizing the usage of expensive metals like platinum. As proof-of-concept, herein it demonstrates that using density functional theory (DFT) calculations and experimental validation that intermetallic PtCo3 alloy nanoparticles offer enhanced electrocatatalytic performance for the oxygen reduction reaction (ORR) compared to Pt nanoparticles. DFT calculations established that PtCo3(111) surfaces possess better intrinsic ORR activity compared to Pt(111) surfaces, owing to the synergistic action of adjacent Pt and Co active sites which optimizes the binding strength of ORR intermediates to boost overall ORR kinetics. With this understanding, a PtCo3/NC catalyst, comprising PtCo3 nanoparticles exposing predominantly (111) facets dispersed on an N-doped carbon support, is successfully fabricated. PtCo3/NC demonstrates a high specific activity (3.4 mA cm-2 mgPt -1), mass activity (0.67 A mgPt -1), and cycling stability for the ORR in 0.1 M KOH, significantly outperforming a commercial 20 wt.% Pt/C catalyst. Moreover, a zinc-air battery (ZAB) assembled with PtCo3/NC as the air-electrode catalyst delivered an open-circuit voltage of 1.47 V, a specific capacity of 775.1 mAh gZn -1 and excellent operation durability after 200 discharge/charge cycles, vastly superior performance to a ZAB built using commercial Pt/C+IrO2 as the air-electrode catalyst.

Facile Construction of CuFe-Based Metal Phosphides for Synergistic NOx -Reduction to NH3 and Zn-Nitrite Batteries in Electrochemical Cell.

The electrocatalytic nitrite/nitrate reduction reaction (eNO2RR/eNO3RR) offer a promising route for green ammonia production. The development of low cost, highly selective and long-lasting electrocatalysts for eNO2RR/eNO3RR is challenging. Herein, a method is presented for constructing Cu3P-Fe2P heterostructures on iron foam (CuFe-P/IF) that facilitates the effective conversion of NO2 - and NO3 - to NH3. At -0.1 and -0.2 V versus RHE (reversible hydrogen electrode), CuFe-P/IF achieves a Faradaic efficiency (FE) for NH3 production of 98.36% for eNO2RR and 72% for eNO3RR, while also demonstrating considerable stability across numerous cycles. The superior performance of CuFe-P/IF catalyst is due tothe rich Cu3P-Fe2P heterstuctures. Density functional theory calculations have shed light on the distinct roles that Cu3P and Fe2P play at different stages of the eNO2RR/eNO3RR processes. Fe2P is notably active in the early stages, engaging in the capture of NO2 -/NO3 -, O─H formation, and N─OH scission. Conversely, Cu3P becomes more dominant in the subsequent steps, which involve the formation of N─H bonds, elimination of OH* species, and desorption of the final products. Finally, a primary Zn-NO2 - battery is assembled using CuFe-P/IF as the cathode catalyst, which exhibits a power density of 4.34 mW cm-2 and an impressive NH3 FE of 96.59%.

Iron-Cobalt Phosphide Encapsulated in a N-Doped Carbon Framework as a Promising Low-Cost Oxygen Reduction Electrocatalyst for Zinc-Air Batteries.

The oxygen reduction reaction (ORR) plays a vital role in many next-generation electrochemical energy conversion and storage devices, motivating the search for low-cost ORR electrocatalysts possessing high activity and excellent durability. In this work, we demonstrate that iron-cobalt phosphide (FeCoP) nanoparticles encapsulated in a N-doped carbon framework (FeCoP@NC) represent a very promising catalyst for the ORR in alkaline media. The core-shell structured FeCoP@NC catalyst offered outstanding ORR activity with a half-wave potential (E1/2) of 0.86 V vs reversible hydrogen electrode (RHE) and excellent stability in a 0.1 M KOH electrolyte, outperforming commercial Pt/C and many recently reported noble-metal-free ORR electrocatalysts. The superiority of FeCoP@NC as an ORR electrocatalyst relative to Pt/C was further verified in prototype zinc-air batteries (ZABs), with the aqueous and flexible ZABs prepared using FeCoP@NC offering excellent stability, impressive open circuit voltages (1.56 and 1.44 V, respectively), and high maximum power densities (183.5 and 69.7 mW cm-2, respectively). Density functional theory calculations revealed that encapsulating FeCoP nanoparticles in N-doped carbon shells resulted in favorable electron penetration effects, which synergistically regulated the adsorption/desorption of ORR intermediates for optimal ORR performance while also boosting the electronic conductivity. Our findings offer valuable new insights for rational design of transition metal phosphide-based catalysts for the ORR and other electrochemical applications.

Palladium(II) Modulation Enhances the Water Stability and Aqueous 99TcO4-/ReO4- Removal Performance of Metal-Organic Frameworks.

Improving the water stability of metal-organic frameworks (MOFs) is essential for their use in water pollution treatment and environmental remediation, though it remains technically challenging. Herein, we report a novel cationic MOF constructed with [Th6O4(OH)4(COO)12] units and [CoN4·Cl2] units possessing a ftw-type topology (denoted as 1-Th-Co). 1-Th-Co itself exhibited poor water stability but excellent stability following a palladium(II) modulation strategy. Experimental studies reveal that Co(II) ions in 1-Th-Co were replaced by Pd(II) ions through cation exchange in N,N-diethylformamide (yielding 1-Th-Pd). The planar PdN4 units in 1-Th-Pd were responsible for improving the water stability of the framework. As a result, 1-Th-Pd offered excellent stability, fast adsorption kinetics, and high removal ratios for 99TcO4- and ReO4- (as a 99TcO4- surrogate) in contaminated water. When used in packed columns, 1-Th-Pd can dynamically capture ReO4- from groundwater. This work provides a new avenue for improving the water stability of MOFs, offering new vistas for the decontamination of aqueous solutions containing 99TcO4- and ReO4-.

Recent advances in the design of afterglow materials: mechanisms, structural regulation strategies and applications.

Afterglow materials are attracting widespread attention owing to their distinctive and long-lived optical emission properties which create exciting opportunities in various fields. Recent research has led to the discovery of many new afterglow materials featuring high photoluminescence quantum yields (PLQY) and lifetimes of up to several hours under ambient conditions. Afterglow materials are typically categorized according to their luminescence mechanism, such as long-persistent luminescence (LPL), room temperature phosphorescence (RTP), or thermally activated delayed fluorescence (TADF). Through rational design and novel synthetic strategies to modulate spin-orbit coupling (SOC) and populate triplet exciton states (T1), luminophores with long lifetimes and bright afterglow characteristics can be realized. Initial research towards afterglow materials focused mainly on pure inorganic materials, many of which possessed inherent disadvantages such as metal toxicity or low energy emissions. In recent years, organic-inorganic hybrid afterglow materials (OIHAMs) have been developed with high PLQY and long lifetimes. These hybrid materials exploit the tunable structure and easy processing of organic molecules, as well as enhanced SOC and intersystem crossing (ISC) processes involving heavy atom dopants, to achieve excellent afterglow performance. In this review, we begin by briefly discussing the structure and composition of inorganic and organic-inorganic hybrid afterglow materials, including strategies for regulating their lifetime, PLQY and luminescence wavelength. The specific advantages of organic-inorganic hybrid afterglow materials, including low manufacturing costs, diverse molecular/electronic structures, tunable structures and optical properties, and compatibility with a variety of substrates, are emphasized. Subsequently, we discuss in detail the fundamental mechanisms used by afterglow materials, their classification, design principles, and end applications (including sensing, anticounterfeiting, and photoelectric devices, among others). Finally, existing challenges and promising future directions are discussed, laying a platform for the design of afterglow materials for specific applications.

Carbon Dot Based Multicolor Electroluminescent LEDs with Nearly 100% Exciton Utilization Efficiency.

Carbon dots (CDs) are promising nanomaterials for next-generation lighting and displays due to their tunable bandgap, high photoluminescence quantum yield (PLQY), and high stability. However, the exciton utilization efficiency (EUE) of CD-based films can only reach 25%, fundamentally limiting their application in electroluminescent light-emitting diodes (LEDs). Improving the EUE is therefore of great significance. Herein, we developed composite films containing CDs and poly(9-vinylcarbazole) (PVK). The films were then used to construct a series of high-performance electroluminescent LEDs with tunable emission colors covering the blue to green regions as the concentration of CDs in the films increased, delivering a maximum external quantum efficiency and current efficiency of 2.62% and 5.11 cd/A, respectively. Theoretical calculations and experiments established that the excellent performance at low film PLQY was due to a hot exciton effect in the CDs, achieving nearly 100% EUE. This work provides new design strategies toward high-performance CD-based electroluminescent LEDs.

Toward More Efficient Carbon-Based Electrocatalysts for Hydrogen Peroxide Synthesis: Roles of Cobalt and Carbon Defects in Two-Electron ORR Catalysis.

Electrochemical production of H2O2 is a cost-effective and environmentally friendly alternative to the anthraquinone-based processes. Metal-doped carbon-based catalysts are commonly used for 2-electron oxygen reduction reaction (2e-ORR) due to their high selectivity. However, the exact roles of metals and carbon defects on ORR catalysts for H2O2 production remain unclear. Herein, by varying the Co loading in the pyrolysis precursor, a Co-N/O-C catalyst with Faradaic efficiency greater than 90% in alkaline electrolyte was obtained. Detailed studies revealed that the active sites in the Co-N/O-C catalysts for 2e-ORR were carbon atoms in C-O-C groups at defect sites. The direct contribution of cobalt single atom sites and metallic Co for the 2e-ORR performance was negligible. However, Co plays an important role in the pyrolytic synthesis of a catalyst by catalyzing carbon graphitization, tuning the formation of defects and oxygen functional groups, and controlling O and N concentrations, thereby indirectly enhancing 2e-ORR performance.

Development of a capillary electrophoresis method based on magnetic solid-phase extraction for simultaneous and sensitive detection of eight biogenic amines in foods.

BACKGROUND: Biogenic amines (BAs) in high concentrations are toxic and may cause a series of health symptoms. A sensitive measurement of BA levels is essential for human health. Capillary electrophoresis (CE) has emerged for the separation of eight BAs due to simple sample preparation and highly efficient separation. However, an important drawback for CE is low sensitivity. Magnetic solid-phase extraction (MSPE) has become a technique of interest owing to its brief operation and low solvent consumption. Hence, MSPE as a pretreatment has great potential to improve CE sensitivity for the analysis of BAs in complex food. RESULTS: Results showed that the Pt-Co-MWCNTs-COOH possessed strong magnetism, good reusability, and high adsorptive ability toward eight biogenic amines based on the hydrogen bonding between the -COOH of Pt-Co-MWCNTs-COOH and -NH2 groups of BAs. Using it as an adsorbent, a magnetic solid-phase extraction coupled with capillary electrophoresis (MSPE-CE) method was developed to effectively extract and sensitively analyze eight BAs. Under optimal conditions, the MSPE-CE method has wide linearities (10.0-1000.0 µg L-1 ) and low limits of detection (1.0-6.1 µg L-1 ). The accuracy of the developed method yielded recovery values from 82.07% to 102.58%. Meanwhile, the BAs contents in two samples were analyzed using the MSPE-CE method, with the results consistent with those detected by a high-performance liquid chromatography method. CONCLUSION: Given those advantages, the established MSPE-CE method promises the practical guidance of monitoring a variety of BAs and provides a foundation for the detection of other food hazards. © 2023 Society of Chemical Industry.

Photocatalytic CO2 Reduction by Near-Infrared-Light (1200 nm) Irradiation and a Ruthenium-Intercalated NiAl-Layered Double Hydroxide.

Near-infrared light-driven photocatalytic CO2 reduction (NIR-CO2PR) holds tremendous promise for the production of valuable commodity chemicals and fuels. However, designing photocatalysts capable of reducing CO2 with low energy NIR photons remains challenging. Herein, a novel NIR-driven photocatalyst comprising an anionic Ru complex intercalated between NiAl-layered double hydroxide nanosheets (NiAl-Ru-LDH) is shown to deliver efficient CO2 photoreduction (0.887 µmol h-1) with CO selectivity of 84.81% under 1200 nm illumination and excellent stability over 50 testing cycles. This remarkable performance results from the intercalated Ru complex lowering the LDH band gap (0.98 eV) via a compression-related charge redistribution phenomenon. Furthermore, transient absorption spectroscopy data verified light-induced electron transfer from the Ru complex towards the LDH sheets, increasing the availability of electrons to drive CO2PR. The presence of hydroxyl defects in the LDH sheets promotes the adsorption of CO2 molecules and lowers the energy barriers for NIR-CO2PR to CO. To our knowledge, this is one of the first reports of NIR-CO2PR at wavelengths up to 1200 nm in LDH-based photocatalyst systems.

Room Temperature Ion Beam Synthesis of Ultra-Fine Molybdenum Carbide Nanoparticles: Toward a Scalable Fabrication Route for Earth-Abundant Electrodes.

Molybdenum carbides are promising low-cost electrocatalysts for electrolyzers, fuel cells, and batteries. However, synthesis of ultrafine, phase-pure carbide nanoparticles (diameter < 5 nm) with large surface areas remains challenging due to uncontrollable agglomeration that occurs during traditional high temperature syntheses. This work presents a scalable, physical approach to synthesize molybdenum carbide nanoparticles at room temperature by ion implantation. By tuning the implantation conditions, various molybdenum carbide phases, stoichiometries, and nanoparticle sizes can be accessed. For instance, molybdenum ion implantation into glassy carbon at 30 keV energy and to a fluence of 9 × 1016 at cm-2 yields a surface η-Mo3 C2 with a particle diameter of (10 ± 1) nm. Molybdenum implantation into glassy carbon at 60 keV to a fluence of 6 × 1016 at cm-2 yields a buried layer of ultrafine γ'-MoC/η-MoC nanoparticles. Carbon ion implantation at 20 keV into a molybdenum thin film produces a 40 nm thick layer primarily composed of ß-Mo2 C. The formation of nanoparticles in each molybdenum carbide phase is explained based on the Mo-C phase diagram and Monte-Carlo simulations of ion-solid interactions invoking the thermal spike model. The approaches presented are widely applicable for synthesis of other transition metal carbide nanoparticles as well.

CuC(O) Interfaces Deliver Remarkable Selectivity and Stability for CO2 Reduction to C2+ Products at Industrial Current Density of 500 mA cm-2.

The electrocatalytic CO2 reduction reaction (CO2 RR) is an attractive technology for CO2 valorization and high-density electrical energy storage. Achieving a high selectivity to C2+ products, especially ethylene, during CO2 RR at high current densities (>500 mA cm-2 ) is a prized goal of current research, though remains technically very challenging. Herein, it is demonstrated that the surface and interfacial structures of Cu catalysts, and the solid-gas-liquid interfaces on gas-diffusion electrode (GDE) in CO2 reduction flow cells can be modulated to allow efficient CO2 RR to C2+ products. This approach uses the in situ electrochemical reduction of a CuO nanosheet/graphene oxide dots (CuOC(O)) hybrid. Owing to abundant CuOC interfaces in the CuOC(O) hybrid, the CuO nanosheets are topologically and selectively transformed into metallic Cu nanosheets exposing Cu(100) facets, Cu(110) facets, Cu[n(100) × (110)] step sites, and Cu+ /Cu0 interfaces during the electroreduction step, the faradaic efficiencie (FE) to C2+ hydrocarbons was reached as high as 77.4% (FEethylene  ≈ 60%) at 500 mA cm-2 . In situ infrared spectroscopy and DFT simulations demonstrate that abundant Cu+ species and Cu0 /Cu+ interfaces in the reduced CuOC(O) catalyst improve the adsorption and surface coverage of *CO on the Cu catalyst, thus facilitating CC coupling reactions.

Regulating the Coordination Geometry and Oxidation State of Single-Atom Fe Sites for Enhanced Oxygen Reduction Electrocatalysis.

FeNC catalysts demonstrate remarkable activity and stability for the oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells and Zn-air batteries (ZABs). The local coordination of Fe single atoms in FeNC catalysts strongly impacts ORR activity. Herein, FeNC catalysts containing Fe single atoms sites with FeN3 , FeN4 , and FeN5 coordinations are synthesized by carbonization of Fe-rich polypyrrole precursors. The FeN5 sites possess a higher Fe oxidation state (+2.62) than the FeN3 (+2.23) and FeN4 (+2.47) sites, and higher ORR activity. Density functional theory calculations verify that the FeN5 coordination optimizes the adsorption and desorption of ORR intermediates, dramatically lowering the energy barrier for OH- desorption in the rate-limiting ORR step. A primary ZAB constructed using the FeNC catalyst with FeN5 sites demonstrates state-of-the-art performance (an open circuit potential of 1.629 V, power density of 159 mW cm-2 ). Results confirm an intimate structure-activity relationship between Fe coordination, Fe oxidation state, and ORR activity in FeNC catalysts.

Recent advances in utilization of pectins in biomedical applications: a review focusing on molecular structure-directing health-promoting properties.

The numerous health benefits of pectins justify their inclusion in human diets and biomedical products. This review provides an overview of pectin extraction and modification methods, their physico-chemical characteristics, health-promoting properties, and pharmaceutical/biomedical applications. Pectins, as readily available and versatile biomolecules, can be tailored to possess specific functionalities for food, pharmaceutical and biomedical applications, through judicious selection of appropriate extraction and modification technologies/processes based on green chemistry principles. Pectin's structural and physicochemical characteristics dictate their effects on digestion and bioavailability of nutrients, as well as health-promoting properties including anticancer, immunomodulatory, anti-inflammatory, intestinal microflora-regulating, immune barrier-strengthening, hypercholesterolemia-/arteriosclerosis-preventing, anti-diabetic, anti-obesity, antitussive, analgesic, anticoagulant, and wound healing effects. HG, RG-I, RG-II, molecular weight, side chain pattern, and degrees of methylation, acetylation, amidation and branching are critical structural elements responsible for optimizing these health benefits. The physicochemical characteristics, health functionalities, biocompatibility and biodegradability of pectins enable the construction of pectin-based composites with distinct properties for targeted applications in bioactive/drug delivery, edible films/coatings, nano-/micro-encapsulation, wound dressings and biological tissue engineering. Achieving beneficial synergies among the green extraction and modification processes during pectin production, and between pectin and other composite components in biomedical products, should be key foci for future research.

The potential of dietary fiber in building immunity against gastrointestinal and respiratory disorders.

The numerous health benefits of dietary fibers (DFs) justify their inclusion in human diets and biomedical products. Given the short- and long-term human impacts of the COVID-19 virus on human health, the potential of DFs in building immunity against gastrointestinal and respiratory disorders is currently receiving high attention. This paper reviews the physicochemical properties of DFs, together with their immune functions and effects on the gastrointestinal tract and respiratory system mainly based on research in the last ten years. Possible modes of action of DFs in promoting health, especially building immunity, are explored. We seek to highlight the importance of understanding the exact physical and chemical characteristics and molecular behaviors of DFs in providing specific immune function. This review provides a perspective beyond the existing recognition of DFs' positive effects on human health, and offers a theoretical framework for the development of special DFs components and their application in functional foods and other therapeutic products against gastrointestinal and respiratory disorders. DFs enhance immunity from gastrointestinal and respiratory diseases to promote host health.

Modulating Anion Nanotraps via Halogenation for High-Efficiency 99TcO4-/ReO4- Removal under Wide-Ranging pH Conditions.

Efficient and sustainable methods for 99TcO4- removal from acidic nuclear waste streams, contaminated water, and highly alkaline tank wastes are highly sought after. Herein, we demonstrate that ionic covalent organic polymers (iCOPs) possessing imidazolium-N+ nanotraps allow the selective adsorption of 99TcO4- under wide-ranging pH conditions. In particular, we show that the binding affinity of the cationic nanotraps toward 99TcO4- can be modulated by tuning the local environment around the nanotraps through a halogenation strategy, thereby enabling universal pH 99TcO4- removal. A parent iCOP-1 possessing imidazolium-N+ nanotraps showed fast kinetics (reaching adsorption equilibrium in 1 min), a high adsorption capacity (up to 1434.1 ± 24.6 mg/g), and exceptional selectivity for 99TcO4- and ReO4- (nonradioactive analogue of 99TcO4-) removal in contaminated water. By introducing F groups near the imidazolium-N+ nanotrap sites (iCOP-2), a ReO4- removal efficiency over 58% was achieved in 60 min in 3 M HNO3 solution. Further, introduction of larger Br groups near the imidazolium-N+ binding sites (iCOP-3) imparted a pronounced steric effect, resulting in exceptional adsorption performance for 99TcO4- under super alkaline conditions and from low-activity waste streams at US legacy Hanford nuclear sites. The halogenation strategy reported herein guides the task-specific design of functional adsorbents for 99TcO4- removal and other applications.