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Triply periodic minimal surfaces (TPMS) inspired by nature serve as a foundation for developing novel nanomaterials, such as templated silicas, graphene sponges, and schwarzites, with customizable optical, poroelastic, adsorptive, catalytic, and other properties. Computer simulations of reactions on TPMS using reactive intermolecular potentials hold great promise for constructing and screening potential TPMS with the desired properties. Here, we developed an off-lattice, surface-constrained Metropolis Monte Carlo (SC-MMC) algorithm that utilized a temperature quench process. The presented SC-MMC algorithm was used to investigate the process of graphitization reactions on the Schwarz primitive, Schwarz diamond, and Schoen gyroid TPMS, all with a cubic lattice parameter of 8 nm. We show that the optimized carbon TPMS exhibits a low energy, approximately -7.1 eV/atom, comparable to that of graphite and diamond crystals, along with a variety of topological defects. Furthermore, these structures showcase extensive and smooth surfaces characterized by a negative discrete Gaussian curvature, a distinctive feature indicative of an interconnected morphology. They possess specific surface areas of â¼2700 m2/g, comparable to graphene, and exhibit a significant porosity of around 90%. The theoretical X-ray correlation functions and nitrogen adsorption isotherms confirm that the constructed TPMS exhibit remarkably similar surface properties, although the pore space topology varies significantly.
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Wetting is very common phenomenon, and it is well documented that the wettability of a solid depends on the surface density of adsorbed airborne hydrocarbons. This "hydrocarbon hypothesis" has been experimentally confirmed for different surfaces, for example, graphene, TiO2, and SiO2; however, there are no scientific reports describing the influence of airborne contaminants on the water contact angle (WCA) value measured on the polytetrafluoroethylene (PTFE) surface. Using experimental data showing the influence of airborne hydrocarbons on the wettability of graphene, gold and PTFE by water, together with Molecular Dynamics simulation results we prove that the relation between the WCA and the surface concentration of hydrocarbons ( n-decane, n-tridecane, and n-tetracosane) is more complex than has been assumed up until now. We show, in contrast to commonly approved opinion, that adsorbed hydrocarbons can increase (graphene, Au) or decrease (PTFE) the WCA of a nanodroplet sitting on a surface. Using classical thermodynamics, a simple theoretical approach is developed. It is based on two adsorbed hydrocarbon states, namely, "carpet" and "dimple". In the "carpet" state a uniform layer of alkane molecules covers the entire substrate. In contrast, in the "dimple" state, the preadsorbed layer of alkane molecules covers only the open surface. Simple thermodynamic balance between the two states explains observed experimental and simulation results, forming a good starting point for future studies.
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The aim of this study is to link polytetrafluoroethylene (PTFE) surface characteristics with its wetting properties in the nanoscale. To do this using molecular dynamics (MD) simulation, three series of rough PTFE surfaces were generated by annealing and compressing and next characterized by the application of the MD version of the atomic force microscopy (AFM) method. The values of specific surface areas were additionally calculated. The TIP4P/2005 water model was used to study the wetting properties of obtained PTFE samples. The simulated water contact angle (WCA) value for the most flat (but slightly rough) sample having PTFE density is equal to 106.94°, and it is close to the value suggested for a perfect PTFE surface on the basis of experimental results. Also, the changes in the WCA with PTFE compression are in the same range as experimentally reported. The obtained MD simulation results make it possible to link, for the first time, the WCA values with the surface MD-AFM root-mean-square roughness and with the PTFE density. Finally, we show that for PTFE wetting in the nanoscale, the line tension is negligible and the Bormashenko's equation reduces to the Cassie-Baxter (CB) model. In fact, our simulation results are close to the CB mechanism.
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Despite extensive research over the last several decades, the microscopic characterization of topological phases of adsorbed phenol from aqueous solutions in carbon micropores (pore size < 2.0 nm), which are believed to exhibit a solid and quasi-solid character, has not been reported. Here, we present a combined experimental and molecular level study of phenol adsorption from neutral water solutions in graphitic carbon micropores. Theoretical and experimental results show high adsorption of phenol and negligible coadsorption of water in hydrophobic graphitic micropores (super-sieving effect). Graphic processing unit-accelerated molecular dynamics simulation of phenol adsorption from water solutions in a realistic model of carbon micropores reveal the formation of two-dimensional phenol crystals with a peculiar pattern of hydrophilic-hydrophobic stripes in 0.8 nm supermicropores. In wider micropores, disordered phenol assemblies with water clusters, linear chains, and cavities of various sizes are found. The highest surface density of phenol is computed in 1.8 nm supermicropores. The percolating water cluster spanning the entire pore space is found in 2.0 nm supermicropores. Our findings open the door for the design of better materials for purification of aqueous solutions from nonelectrolyte micropollution.
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The new molecular dynamics simulation results showing the influence of the edge carbon surface atoms on the wettability of a highly oriented pyrolytic graphite (HOPG) surface with water nanodroplets are reported. The conditions for the occurrence of the Wenzel effect are discussed, and the Cassie-to-Wenzel transition (CTWT) mechanism in the nanoscale is explored. This transition is detected by the application of a new procedure showing that the CTWT point shifts toward larger values of carbon-oxygen potential well depth with the decrease in the HOPG side angle. It is concluded that the Wenzel effect significantly contributes to the contact angles (CAs) measured for the HOPG surfaces. The Wenzel effect is also very important for the "HOPG" structures possessing the disturbed C-C interlayer distance, and its influence on the water nanodroplet CAs is strongly pronounced. The structure of water confined inside slits and on a HOPG surface is studied using the analysis of the density profiles, the number of hydrogen bonds, and, modified for the purpose of this study, structure factor. The detailed analysis of all parameters describing confined water leads to the conclusion about the presence of characteristic interference patterns revealed as a result of long-term simulation. A simple model describing this effect is proposed as the starting point for further considerations.
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The detonation nanodiamonds form the aggregate having interparticle voids, giving a marked hygroscopic property. As the relationship between pore structure and water adsorption of aggregated nanodiamonds is not well understood yet, adsorption isotherms of N2 at 77 K and of water vapor at 298 K of the well-characterized aggregated nanodiamonds were measured. HR-TEM and X-ray diffraction showed that the nanodiamonds were highly crystalline and their average crystallite size was 4.5 nm. The presence of the graphitic layers on the nanodiamond particle surface was confirmed by the EELS examination. The pore size distribution analysis showed that nanodiamonds had a few ultramicropores with predominant mesopores of 4.5 nm in average size. The water vapor adsorption isotherm of IUPAC Type V indicates the hydrophobicity of the nanodiamond aggregates, with the presence of hydrophilic sites. Then the hygroscopic nature of nanodiamonds should be associated with the surface functionalities of the graphitic shell and the ultramicropores on the mesopore walls.
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In this study, graphene oxide (GO) has been applied as a matrix for enzyme immobilization. The protein adsorption capacity of GO is much higher than of other large surface area carbonaceous materials. Its structure and physicochemical properties are reported beneficial also for enzymatic activity modifications. The experimental proof was done here that GO-based biocatalytic systems with immobilized catalase are modifiable in terms of catalyzed reaction kinetic constants. It was found that activity and stability of catalase, considered here as model enzyme, closely depend on enzyme/GO ratio. The changes in kinetic parameters can be related to secondary structure alterations. The correlation between enzyme/GO ratio and kinetic and structure parameters is reported for the first time and enables the conscious control of biocatalytic processes and their extended applications. The biological activity of obtained biocatalytic systems was confirmed in vitro by the use of functional test. The addition of immobilized catalase improved the cells' viability after they were exposed to hydrogen peroxide and tert-butyl-hydroperoxide used as source of reactive oxygen species.
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Catalasa/metabolismo , Enzimas Inmovilizadas/metabolismo , Grafito/química , Animales , Biocatálisis , Células CHO , Catalasa/química , Supervivencia Celular/efectos de los fármacos , Cricetulus , Activación Enzimática , Estabilidad de Enzimas , Enzimas Inmovilizadas/química , Peróxido de Hidrógeno/farmacología , Cinética , Estructura Secundaria de Proteína , terc-Butilhidroperóxido/farmacologíaRESUMEN
Pillared graphene structures, from a practical viewpoint, are very interesting novel carbon materials. Combining the properties of graphene and nanotubes, such as durability, chemical purity and a controlled structure, they were proven to be effective membranes for noble gas separation processes. Here, we examine their possible use for other, more commercially useful gas mixture separation, i.e. air and coal gas. The mechanism of air gas transport through the pillar channels is studied, and the prospective application of 2-D pillared membranes in effusion-like processes provided. The separative abilities of hybrid systems consisting of membranes with different channel diameters in relation to coal gas are proven to be promising.
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A series of porous carbon matrixes was prepared by phosphoric (V) acid activation of unconventional precursors chitin and chitosan: impregnation with H3PO4 at concentrations ranging from 1.34 to 5.53 mole dm(-3), followed by carbonization at 600 degrees C. The obtained carbons demonstrated well-developed porosity that declined steadily in the micropore and mesosopore ranges, depending on both the kind of the precursor and the concentration of activator. The surface area and pore volume of the carbons prepared from chitin increased upon the rising impregnation ratio. The surface area and total pore volume reached their maximum values (1257 m2g(-1) and 1.007 cm3g(-1), respectively) for the acid concentration of 3.40 mole dm(-3). The chars obtained from chitosan showed the values of the BET surface area ranging from 970 to 1484 m2g(-1). Chemical analysis indicated that the activation with phosphoric acid led to the chars of exceptionally high concentration of nitrogenated functionalities and a typical amount of oxygenated surface groups.
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Carbono/química , Quitina/química , Quitosano/química , Nanoestructuras , Microscopía Electrónica de Rastreo , Espectroscopía de Fotoelectrones , Porosidad , Espectrometría por Rayos XRESUMEN
The GCMC technique is used for simulation of adsorption of CO2-CH4, CO2-N2 and CH4-N2 mixtures (at 298 K) on six porous carbon models. Next we formulate a new condition of the IAS concept application, showing that our simulated data obey this condition. Calculated deviations between IAS predictions and simulation results increase with the rise in pressure as in the real experiment. For the weakly adsorbed mixture component the deviation from IAS predictions is higher, especially when its content in the gas mixture is low, and this is in agreement with the experimental data. Calculated activity coefficients have similar plots to deviations between IAS and simulations, moreover obtained from simulated data activity coefficients are similar qualitatively as well as quantitatively to experimental data. Since the physical interpretation of activity coefficients is completely lacking we show for the first time that they can be described by the formulas derived from the expression for G(ex) for the ternary mixture. Finally we also for the first time show the linear relationship between the chemical potentials of nonideal and ideal solutions and the reduced temperature of interacting mixture components, and it is proved that the deviation from ideality is larger if adsorption occurs in a more microporous system.
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We present the first in silico modeling of the Pd-H-single-walled carbon nanohorn nanocomposites. Temperature-quench Monte Carlo simulations are used to generate the most stable morphologies of Pd81 clusters (cluster sizes of â¼2 nm) deposited inside the morphologically defective single-walled carbon nanohorns (S. Furmaniak, A. P. Terzyk, K. Kaneko, P. A. Gauden, P. Kowalczyk, T. Itoh, Phys. Chem. Chem. Phys., 2013, 15, 1232-1240). The optimized Pd81-single-walled carbon nanohorn nanocomposites are next used in calculating the H binding energy distributions at 300 K. The most stable positions of H impurity in confined Pd81 clusters are identified, showing subsurface character of H absorption from the dilute H2 gas at 300 K. The H binding energy distribution on the Pd(100) open surface at 300 K is computed and compared with those corresponding to Pd81-single-walled carbon nanohorn nanocomposites. Finally, the impact of the Pd-H short-range order on the H binding energy is explored and critically discussed.
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Carbon nanoallotropes have attracted significant attention in the field of materials science due to their unique combination of physicochemical and biological properties, with numerous applications. One-dimensional (1D) and two-dimensional (2D) sp2-carbon nanoallotropes, such as carbon nanohorns (CNHs), carbon nanotubes (CNTs), and graphene, have emerged as prominent candidates for a variety of technological advancements. To fully exploit their exceptional characteristics, the covalent functionalization of these nanostructures may alleviate the problems with the processing and final performance. This route of the carbon nanoallotrope functionalization is based on a covalent attachment of functional groups or molecules (via linkers of various strengths) to their surfaces, enabling precise control over physical, chemical, biological, and electronic properties. Such an approach opens up new avenues for tailoring the nanoallotrope characteristics, such as solubility/dispersibility, reactivity, and interactions with other materials. Over more than the last decade, significant progress has been made in the covalent functionalization of both 1D and 2D sp2-carbon nanoallotropes, paving the way for diverse applications in the nanoelectronics, energy storage, sensing, and biomedical fields. In this comprehensive review, we provide state-of-the-art advancements and achievements in the covalent functionalization of 1D and 2D sp2-carbon nanoallotropes during the past dozen years. We aim to highlight the key strategies, methodologies, and breakthroughs that have significantly contributed to this field. Eventually, we discuss the implications of those advancements and explore the opportunities for future research and applications.
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Using realistic models of single-walled carbon nanohorns and their single-walled carbon nanotube counterparts, we study the equilibrium separation of CO2-CH4 mixtures near ambient operating conditions by using molecular simulations. We show that regardless of the studied operating conditions (i.e., total CO2-CH4 mixture pressures and mole fractions of mixture components in the bulk phase), single-walled carbon nanohorns maximize the CO2-CH4 equilibrium separation factor. Optimized samples of single-walled carbon nanohorns consisting of narrow tubular parts capped with horn-shaped tips show highly selective adsorption of CO2 over the CH4 mixture component, with the CO2-CH4 equilibrium separation factor of ~8-12. A large surface-to-volume ratio (i.e., enhanced surface forces) and unique defective morphology (i.e., packing of adsorbed molecules in quasi-one/quasi-zero dimensional nanospaces) of single-walled carbon nanohorns are their key structural properties responsible for the excellent separation performance. Our theoretical simulation results are in quantitative agreement with a recent experimental/theoretical study of the CO2-CH4 adsorption and separation on oxidized single-walled carbon nanohorns [Ohba et al., Chem. Lett., 40, 2011, 1089]. Both experiment and theory showed that the CO2-CH4 equilibrium separation factor of oxidized samples of single-walled nanohorns measured near ambient operating conditions is ~2-5. This reduction in the separation efficiency as compared to optimized samples of single-walled carbon nanohorns is theoretically justified by their lower surface-to-volume ratio (i.e., larger diameters of tubular parts and horn-shaped tips).
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Dióxido de Carbono/química , Técnicas de Química Analítica/métodos , Metano/química , Nanotubos de Carbono/química , Simulación por Computador , Propiedades de SuperficieRESUMEN
A strategy for combined experimental and computational screening of candidate carbonaceous materials for capturing highly volatile nerve agents at ambient temperature using physisorption. Based on theoretical calculations of Henry constants and zero-coverage adsorption enthalpies for sarin and DMMP (its common stimulant) adsorbed in model slit-shaped carbon pores at 298 K, we found the following. Slit-shaped carbon pores with pore width ~0.5 nm are optimal for agent adsorption due to strong confinement of adsorbed molecules. Agent adsorption enthalpy at zero coverage computed for optimal pore width is very high and reaches ~83 kJ mol(-1). Widening of pore width above ~1 nm results in a significant decrease of the Henry constant and zero-coverage adsorption enthalpy (~44 kJ mol(-1)). Polydispersity of studied candidate carbonaceous materials strongly affects adsorption capacity for DMMP under the operating conditions. The optimal carbonaceous adsorbent, pitch-based P7 activated carbon fiber, adsorbed ~100 µg g(-1) DMMP at 0.03 µg m(-3). Commercial Norit activated carbon adsorbed only ~20 µg g(-1) DMMP at 0.03 µg m(-3). Surprisingly, a small shift of the pore size distribution towards wider micropores has a great impact on agent adsorption. Because the adsorption enthalpies computed at zero coverage weakly dependent on pore size, the heat released during agent adsorption is similar for all studied candidate adsorbents (i.e.~55-60 kJ mol(-1)).
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Applying pore size analysis, Monte Carlo simulations, and transition state theory, we study the molecular sieving properties of recently discovered crystalline exotic cubic carbon allotropes (Hu et al., J. Phys. Chem. C, 2012, 116, 24233-24238) at 298 K and infinite dilution. The fcc-C10 cubic carbon crystal shows unusual molecular sieving characteristics. The carbon cavities of the fcc-C10 cubic carbon polymorph (with an effective size of ~3.5-4 Å) are kinetically closed to common gaseous contaminants of He fluid (including: Ne, Ar, H2, and CO). Because the sizes of nanowindows connecting carbon cavities are comparable with the effective size of a He atom (~2.556 Å), we predict a significant resistance to self-diffusion of the He in the fcc-C10 crystal. Computed self-diffusion coefficients ~1.3 × 10(-6)-1.3 × 10(-7) cm(2) s(-1) for He inside fcc-C10 fall in the range characteristic of molecular diffusion in zeolites. Infrequent "jumps" of He atoms between neighboring carbon cavities and kinetic rejection of other gaseous particles indicate potential application of the fcc-C10 carbon polymorph for kinetic molecular sieving of He near ambient temperatures. The theoretical results presented here are useful for correct interpretation of the pore volumes of carbon molecular sieves measured from helium porosimetry.
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A new modelling-aided approach for the atomistic model of single walled carbon nanohorn (SWNH) creation is presented, based on experimental evidence, on realistic potential of carbon-carbon interactions and on molecular simulations. A new model of SWNHs is next used to predict Ar adsorption properties and to check the molecular fundamentals of the adsorption mechanism. The influence of the apex angle value, nanohorn diameter and nanohorn length on the shapes of isotherms, enthalpy, high resolution α(s)-plots and adsorption potential distribution curves is checked. Finally the comparison with new experimental Ar adsorption results is shown and the conclusions on the porosity of real SWNH aggregates are given.
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Nanotubos de Carbono/química , Adsorción , Argón/química , Modelos QuímicosRESUMEN
Introduction: Plant pathogenic microorganisms adversely affect the growth and yield of crops, which consequently leads to losses in food production. Metal-based nanoparticles (MNPs) can be a remedy to solve this problem. Methods: Novel silver nanoparticles (AgNPs) and zinc oxide nanoparticles (ZnONPs) were biosynthesized from Fusarium solani IOR 825 and characterized using Dynamic Light Scattering (DLS), Fourier Transform Infrared (FTIR) spectroscopy, Transmission Electron Microscopy (TEM), X-ray diffraction (XRD) and measurement of Zeta potential. Antibacterial activity of NPs was evaluated against four plant pathogenic strains by determination of the minimum inhibitory (MIC) and biocidal concentrations (MBC). Micro-broth dilution method and poisoned food technique were used to assess antifungal activity of NPs against a set of plant pathogens. Effect of nanopriming with both types of MNPs on maize seed germination and seedlings growth was evaluated at a concentration range of 1-256 µg mL-1. Results: Mycosynthesis of MNPs provided small (8.27 nm), spherical and stable (zeta potential of -17.08 mV) AgNPs with good crystallinity. Similarly, ZnONPs synthesized by using two different methods (ZnONPs(1) and ZnONPs(2)) were larger in size (117.79 and 175.12 nm, respectively) with Zeta potential at -9.39 and -21.81 mV, respectively. The FTIR spectra showed the functional groups (hydroxyl, amino, and carboxyl) of the capping molecules on the surface of MNPs. The values of MIC and MBC of AgNPs against bacteria ranged from 8 to 256 µg mL-1 and from 512 to 1024 µg mL-1, respectively. Both types of ZnONPs displayed antibacterial activity at 256-1024 µg mL-1 (MIC) and 512-2048 µg mL-1 (MBC), but in the concentration range tested, they revealed no activity against Pectobacterium carotovorum. Moreover, AgNPs and ZnONPs inhibited the mycelial growth of Alternaria alternata, Fusarium culmorum, Fusarium oxysporum, Phoma lingam, and Sclerotinia sclerotiorum. MIC and MFC values of AgNPs ranged from 16-128 and 16-2048 µg mL -1, respectively. ZnONPs showed antifungal activity with MIC and MFC values of 128-2048 µg mL-1 and 256-2048 µg mL-1, respectively. The AgNPs at a concentration of ≥32 µg mL-1 revealed sterilization effect on maize seeds while ZnONPs demonstrated stimulatory effect on seedlings growth at concentrations of ≥16 µg mL-1 by improving the fresh and dry biomass production by 24% and 18%-19%, respectively. Discussion: AgNPs and ZnONPs mycosynthesized from F. solani IOR 825 could be applied in agriculture to prevent the spread of pathogens. However, further toxicity assays should be performed before field evaluation. In view of the potential of ZnONPs to stimulate plant growth, they could be crucial in increasing crop production from the perspective of current food assurance problems.
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Herein, we report the functionalization of carbon nano-onions (CNOs) with the hydroxyaryl group and subsequent modifications with resins: resorcinol-formaldehyde using porogenic Pluronic F-127, resorcinol-formaldehyde-melamine, benzoxazine made of bisphenol A and triethylenetetramine, and calix[4]resorcinarene-derived using F-127. Following the direct carbonization, extensive physicochemical analysis was carried out, including Fourier transform infrared, Raman and X-ray photoelectron spectroscopy, scanning and transmission electron microscopy, and adsorption-desorption of N2. The addition of CNO to the materials significantly increases the total pore volume (up to 0.932 cm3 g-1 for carbonized resorcinol-formaldehyde resin and CNO (RF-CNO-C) and 1.242 cm3 g-1 for carbonized resorcinol-formaldehyde-melamine resin and CNO (RFM-CNO-C)), with mesopores dominating. However, the synthesized materials have poorly ordered domains with some structural disturbance; the RFM-CNO-C composite shows a more ordered structure with amorphous and semi-crystalline regions. Subsequently, cyclic voltammetry and galvanostatic charge-discharge method studied the electrochemical properties of all materials. The influence of resins' compositions, CNO content, and amount of N atoms in carbonaceous skeleton on the electrochemical performance was studied. In all cases, adding CNO to the material improves its electrochemical properties. The carbon material derived from CNO, resorcinol and melamine (RFM-CNO-C) showed the highest specific capacitance of 160 F g-1 at a current density of 2 A g-1, which is stable after 3000 cycles. The RFM-CNO-C electrode retains approximately 97% of its initial capacitive efficiency. The electrochemical performance of the RFM-CNO-C electrode results from the hierarchical porosity's stability and the presence of nitrogen atoms in the skeleton. This material is an optimal solution for supercapacitor devices.
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The design of shielding materials against ionizing radiation while simultaneously displaying enhanced multifunctional characteristics remains challenging. Here, for the first time, we present moldable paraffin-based iron nano- and microcomposites attenuating γ- and X-radiation. The moldability was gained by the warmth-of-hands-driven plasticity, which allowed for obtaining a specific shape of the composites at room temperature. The manufactured composites contained iron particles of various sizes, ranging from 22 nm to 63 µm. The target materials were widely characterized using XRD, NMR, Raman, TGA, SEM, and EDX. In the case of microcomposites, the shielding properties were developed at two concentrations: 10 and 50 wt %. The statistically significant results indicate that the iron particle size has a negligible effect on the shielding properties of the nano- and microcomposites. On the other hand, the higher iron particle contents significantly affected the attenuating ability, which emerged even as superior to the elemental aluminum in the X-ray range: at a 70 kV anode voltage, the half value layer was 6.689, 1.882, and 0.462 cm for aluminum, paraffin + 10 wt % Fe 3.5-6.5 µm, and paraffin + 50 wt % Fe 3.5-6.5 µm microcomposites, respectively. Importantly, the elaborated methodology-in situ cross-verified in the hospital studies recording real-life sampling-opens the pathway to high-performance, eco-friendly, lightweight, and recyclable shields manufactured via fully reproducible and scalable protocols.
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Covalent triazine-based frameworks have attracted much interest recently due to their high surface area and excellent thermal and electrochemical stabilities. This study shows that covalently immobilizing triazine-based structures on spherical carbon nanostructures results in the organization of micro- and mesopores in a three-dimensional manner. We selected the nitrile-functionalized pyrrolo[3,2-b]pyrrole unit to form triazine rings to construct a covalent organic framework. Combining spherical carbon nanostructures with the triazine framework produced a material with unique physicochemical properties, exhibiting the highest specific capacitance value of 638 F g-1 in aqueous acidic solutions. This phenomenon is attributed to many factors. The material exhibits a large surface area, a high content of micropores, a high content of graphitic N, and N-sites with basicity and semi-crystalline character. Thanks to the high structural organization and reproducibility, and remarkably high specific capacitance, these systems are promising materials for use in electrochemistry. For the first time, hybrid systems containing triazine-based frameworks and carbon nano-onions were used as electrodes for supercapacitors.