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Two metal-free birefringent crystals, C10H8BrNO2 and C10H8BrNO2·H2O, which contain a new birefringence-active [C10H8NO2]+ gene, were synthesized via a mild solution evaporation method. In their crystal structures, the π-conjugated naphthalene-like [C10H8NO2]+ groups are basically aligned, which induces high optical anisotropy; i.e., the title compounds exhibit large birefringences of 0.36 and 0.41 at 550 nm according to first-principles calculations. Moreover, the UV-vis-near-IR diffuse-reflectance spectra suggest that they have similar optical band gaps. Structural analysis and theoretical calculations show that the [C10H8NO2]+ unit is responsible for the good optical anisotropy. These results make the naphthalene-like motif a good structural gene to search for new birefringent crystals.
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Reversible phase transformations (RPTs) of metal-organic frameworks not only create material diversity but also promise a self-restoration of crystals in a controllable manner. However, there are only limited examples because seeking for a convenient and effective trigger for RPTs, especially for RPTs with respect to spatiotemporal harmony in cleavage and reconstruction of metal-linker chemical bonds, is challenging. In this work, we found that zeolitic imidazolate framework (ZIF)-108 with Zn-N coordination bonds showing moderate strength was an ideal platform. We reported three crystal phases of ZIF-108, namely, sodalite (SOD), diamondoid (DIA), and large pore_sodalite (lp_SOD) topologies, and identified RPTs between phases: (1) when exposed to water or water vapor, the SOD structure could transform to a compact DIA version as a result of the decomposition of four-membered rings and synchronous reorganization of six-membered rings. Then, the DIA structure could also return back to SOD when soaked in dimethylformamide (DMF) or DMF vapor. (2) High-temperature treatment of SOD gives rise to lp_SOD, which then reverts to SOD by DMF. (3) lp_SOD could also be compressed into the DIA phase by water or water vapor and can then be restored via a two-step treatment, namely, soaking in DMF (DIA â SOD) right before a high-temperature therapy (SOD â lp_SOD). From the perspective of the separation utility, we found that the lp_SOD version of ZIF-108, relative to SOD-structured ZIF-108, can produce mixed matrix membranes having an interesting interfacial structure with the polymer chains, though both share the same chemical composition. We verified that the large pore of lp_SOD can allow being penetrated by polymer chains, which contributed to not only reinforcing the bi-phase interface but also sharpening the molecule sieve properties of fillers toward CO2 and CH4.
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Zeolitas , Zeolitas/química , Vapor , Imidazoles/química , Polímeros , GasesRESUMEN
SO4 tetrahedral groups have weak polarization anisotropy, which thus results in the small birefringence of sulfates. Here, we report new sulfate CsY(SO4)2·4H2O with unprecedented birefringence among deep-ultraviolet (deep-UV) sulfates. Its single crystal (10 mm × 3.5 mm × 1.5 mm) was simply grown by an aqueous solution evaporation technique, and it features a rare layered structure composed of YO9 polyhedra, SO4 tetrahedra, and H2O molecules. Interestingly, each SO4 group donates two oxygen atoms to edge-share with one adjacent YO9 polyhedron and thus causes severe distortion of these groups. The characteristic edge-sharing mode gives CsY(SO4)2·4H2O a large birefringence of â¼0.045@546 nm, which is the maximum among deep-UV sulfates and phosphates with similar non-π-conjugated anionic groups. The ultraviolet-visible-near-infrared diffuse reflection and transmission spectra, infrared spectrum, thermal stability, and theoretical calculations are also presented. The fascinating results will improve our understanding of sulfates and may provide useful insights into the exploration of deep-UV sulfates with large birefringence.
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Two-dimensional (2D) materials have attracted extensive attention owing to their unique electronic/physiochemical properties, and wide application potential in energy storage and conversion. However, 2D materials are often tendency to aggregate due to the strong van der Waals interactions, leading to gradually decrease of an efficient mass transfer pathway and accessible surface area for the electrolyte. Here, we demonstrate an efficient approach for large-scale production of a hybrid nanostructures (Ti3C2Tx/rGO) based on ultrathin MXene nanosheets anchored on layered reduced graphene (rGO) supported by porous Ni-foam via a plain chemical dipping method followed by high temperature annealing process. Ti3C2Tx/rGO electrode exhibits a porous structure, excellent ionic and electrical conductivities, and remarkable specific capacitance. Furthermore, it shows ultra-high cycle stability, for example, 88.70% of its specific capacity can be maintained through 3000 cycles. This kind of porous nanostructure and integrated design idea is significant to design other energy storage modules.
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Development of simple and accurate methods for the detection of As3+is highly desirable and technically important. In this work, a highly sensitive and selective long-period fiber gratings sensor based on surface plasmon resonance was developed for As3+detection by designing glutathione-functionalized Au nanoparticles as a signal amplification tag. Based on the chemical interaction between As3+and glutathione, the self-assembling glutathione on the surface of the gold film combines selectively with As3+, and then anchors the glutathione-functionalized Au nanoparticles, which changes the refractive index of the surrounding environment, resulting in a shift of the transmission spectrum. Results show that the sensor could detect As3+with concentrations ranging from 0.02 to 2 ppb. The sensor exhibited excellent specificity for As3+against other metal ions, such as Na+, Fe3+, Mg2+, Cu2+, Pb2+, Ni2+, Ba2+, and Co3+. The fiber sensor was successfully employed to detect As3+in pond water samples, demonstrating that it has the potential for As3+detection with the advantages of low cost, high sensitivity, and a simple structure.
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We orderly assembled zero-dimensional 2-methylimidazole (mim) molecules into unprecedented supramolecule array membranes (SAMs) through solvent-free vapor processing, realizing the intermolecular spacing of mim at ca. 0.30â nm available as size-sieving channels for distinguishing the tiny difference between H2 (kinetic diameter: 0.289â nm) and CO2 (kinetic diameter: 0.33â nm). The highly oriented and dense membranes yield a separation factor above 3600 for equimolar H2 /CO2 mixtures, which is one order of magnitude higher than those of the state-of-the-art membranes defining 2017's upper bound for H2 /CO2 separation. These SAMs define a new benchmark for molecular sieve membranes and are of paramount importance to precombustion carbon capture. Given the range of supramolecules, we anticipate SAMs with variable intermolecular channels could be applied in diversified separations that are prevalent in chemical processes.
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Capture of high-boiling-point furfural from diluted aqueous solution is a critical but challenging step in sustainable bio-refinery processes, but conventional separation methods such as distillation and liquid-liquid extraction requires prohibitive energy consumption. We report control over the microenvironment of hydrated MIL-53 and isoreticular variants with diversified functional terephthalic acid linkers for the purpose of preferential binding of furfural through delicate host-guest interactions. Methyl-bounded MIL-53 with improved binding energy in the hydrated form results in highly efficient capture ratio (ca. 98 %) in the extremely low concentration of furfural solution (0.5-3â wt %) and 100 % furfural specificity over xylose. The distinct hydrogen bonding sites and multiple Van de Wall interactions for furfural adsorption was testified by computational modeling. Furthermore, the recovery ratio of furfural reaches ca. 93 % in desorption.
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The realization of reducing concrete self-weight is mainly to replace ordinary aggregates with lightweight aggregates; such replacement usually comes with some intrinsic disadvantages in concrete, such as high brittleness and lower mechanical properties. However, these shortages can be effectively remedied by external confinement such as fiber reinforced polymer (FRP) jacketing. To accurately predict the stress-strain behavior of lightweight concrete with lateral confinement, it is necessary to properly understand the coupling effects that are caused by diverse aggregates types and confinement level. In this study, FRP-confined lightweight concrete cylinder with varying aggregate types were tested under axial compression. Strain gauges and linear variable displacement transducers were used for monitoring the lateral and axial deformation of specimens during the tests. By sensing the strain and deformation data for the specimens under the tri-axial loads, the results showed that the lateral to axial strain relation is highly related to the aggregate types and confinement level. In addition, when compared with FRP-confined normal weight aggregate concrete, the efficiency of FRP confinement for lightweight concrete is gradually reduced with the increase of external pressure. Replace ordinary fine aggregate by its lightweight counterparts can be significantly improved the deformation capacity of FRP-confined lightweight concrete, meanwhile does not lead to the reduction of compressive strength. Plus, this paper modified a well-established stress-strain model for an FRP-confined lightweight concrete column, involving the effect of aggregate types. More accurate expressions pertaining to the deformation capacity and the stress-strain relation were proposed with reasonable accuracy.
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1-Deoxynojirimycin (DNJ, C6H13NO4, 163.17 g/mol), an alkaloid azasugar or iminosugar, is a biologically active natural compound that exists in mulberry leaves and Commelina communis (dayflower) as well as from several bacterial strains such as Bacillus and Streptomyces species. Deoxynojirimycin possesses antihyperglycemic, anti-obesity, and antiviral features. Therefore, the aim of this detailed review article is to summarize the existing knowledge on occurrence, extraction, purification, determination, chemistry, and bioactivities of DNJ, so that researchers may use it to explore future perspectives of research on DNJ. Moreover, possible molecular targets of DNJ will also be investigated using suitable in silico approach.
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1-Desoxinojirimicina/administración & dosificación , 1-Desoxinojirimicina/aislamiento & purificación , Bacillus/química , Morus/química , Streptomyces/química , 1-Desoxinojirimicina/química , 1-Desoxinojirimicina/farmacología , Fármacos Antiobesidad/administración & dosificación , Fármacos Antiobesidad/aislamiento & purificación , Fármacos Antiobesidad/farmacología , Antivirales/administración & dosificación , Antivirales/aislamiento & purificación , Antivirales/farmacología , Cromatografía Líquida de Alta Presión , Humanos , Hipoglucemiantes/administración & dosificación , Hipoglucemiantes/aislamiento & purificación , Hipoglucemiantes/farmacología , Estructura Molecular , Hojas de la Planta/químicaRESUMEN
Recycled aggregate concrete (RAC) possesses different mechanical properties than ordinary concrete because of inherent faults in recycled aggregates (RAs), such as the old interfacial transition zone (ITZ). However, the application of nano-SiO2 presents an effective methodology to enhance the quality of RA. In this study, nano-SiO2-modified recycled aggregate (SRA) was used to replace natural aggregate (NA), and the stress-strain relationships and cyclic behavior of nano-SiO2-modified recycled aggregate concrete (SRAC) with different SRA replacement rates were investigated. After evaluating the skeleton curve of SRAC specimens, the existing constitutive models were compared. Additionally, the study also proposed a stress-strain model designed to predict the mechanical behavior of concrete in relation to the SRA replacement rate. The results show that compared with RAC, the axial compressive strength of SRAC specimens showed increases of 40.27%, 29.21%, 26.55%, 16.37%, and 8.41% at specific SRA replacement rates of 0%, 30%, 50%, 70%, and 100%, respectively. Moreover, the study found that the Guo model's calculated results can accurately predict the skeleton curves of SRAC specimens.
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The poor performance of recycled concrete aggregate (RCA) leads to greater creep in recycled aggregate concrete (RAC) compared to natural aggregate concrete (NAC). To enhance the quality of RCA, this paper utilizes a 2% concentration of a nano-SiO2 (NS) solution for pre-soaking RCA. This study aims to replace natural aggregate (NA) with NS-modified recycled aggregate (SRCA) and investigate the creep and shrinkage properties of NS-modified recycled aggregate concrete (SRAC) at various SRCA replacement rates. Subsequently, the creep and shrinkage strains of NAC, SRAC, and RAC are simulated using the finite element method. Finally, a comparative analysis is conducted with the predicted creep and shrinkage strains from CEB-FIP, ACI, B3, and GL2000 models. The experimental results indicate that the creep and shrinkage deformation of SRAC increases with the SRCA replacement rate. Compared to NAC, the creep and shrinkage deformation of SRAC at replacement rates of 30%, 50%, 70%, and 100% increased by 2%, 7%, 13%, and 30%, respectively. However, when 100% of the natural aggregate is replaced with SRCA, the creep and shrinkage deformation decreases by 7% compared to RAC. Moreover, the CEB-FIP and ACI models can predict the creep and shrinkage deformation of concrete reasonably well.
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Metal-Organic Framework (MOF) membranes act as selective layers have offered unprecedented opportunities for energy-efficient and cost-effective gas separation. Searching for the green and sustainable synthesis method of dense MOF membrane has received huge attention in both academia and industry. In this work, we demonstrate an in situ electrochemical potential-induced synthesis strategy to aqueously fabricate Metal Azolate Framework-4 (MAF-4) membranes on polypropylene (PP) support. The constant potential can induce the heterogeneous nucleation and growth of MAF-4, resulting an ultrathin membrane with the thickness of only 390 nm. This high-quality membrane exhibits a high H2/CO2 separation performance with the H2 permeance as high as 1565.75 GPU and selectivity of 11.6. The deployment of this environment friendly one-step fabrication method under mild reaction conditions, such as low-cost polymer substrate, water instead of organic solvent, room temperature and ambient pressure shows great promise for the scale-up of MOF membranes.
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In this study, sustainable engineered cementitious composites (ECC) exhibiting high tensile strength as well as high tensile strain capacity were successfully developed by incorporating polyethylene (PE) fiber, local recycled fine aggregate (RFA), and limestone calcined clay cement (LC3). The improvement in tensile strength and tensile ductility was attributed to the self-cementing properties of RFA as well as the pozzolanic reaction between calcined clay and cement. Carbonate aluminates were also generated owing to the reaction between calcium carbonate in limestone and the aluminates in both calcined clay and cement. The bond strength between fiber and matrix was also enhanced. At the age of 150 days, the tensile stress-strain curves of ECC containing LC3 and RFA shifted from a bilinear model to a trilinear model, and the hydrophobic PE fiber exhibited hydrophilic bonding performance when embedded in RFA-LC3-ECC matrix, which could be explained by the densified cementitious matrix as well as the refined pore structure of ECC. Moreover, the substitution of ordinary Portland cement (OPC) by LC3 resulted in energy consumption and equivalent CO2 emission reduction ratios of 13.61% and 30.34%, respectively, when the replacement ratio of LC3 is 35%. Therefore, PE fiber-reinforced RFA-LC3-ECC demonstrates excellent mechanical performance as well as considerable environmental benefits.
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Under the background of climate change, the steel industry is considered one of the least eco-friendly industries. Flax fiber-reinforced polymer (FFRP) is an emerging sustainable alternative to steel reinforcement bar; however, its application is much restricted due to its interior material properties. This paper proposed a novel way to form closed-shape stirrups with FFRP, which is suitable for replacing steel stirrups. A multi-disciplinary investigation was conducted concerning the structural and environmental performance of FFRP stirrups in reinforced concrete (RC) beams. Seven specimens were tested under a three-point bending load. The FFRP stirrups substantially increased the shear capacity and ultimate vertical displacement by 77% and 74%, respectively, and shifted brittle failure to ductile failure. The closed-shape stirrups avoided the stress concentration and increased the utilization of FFRP tensile capacity to over 80%. Decreasing the spacing of FFRP stirrups effectively increased the shear capacity and ductility; increasing the width or layer of FFRP stirrups improved ductility only. A life cycle assessment (LCA) was later performed to evaluate and compare the environmental performance of steel, FFRP, and carbon FRP stirrups. As compared to carbon FRP and steel ones, FFRP stirrups substantially decreased the global warming and fossil depletion potential by over 60%. The main contributors to the environmental impacts of FFRP stirrups were the heavy metal released into the water and terrestrial environment during the cultivation process.
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Fiber-reinforced polymer (FRP) composites have been used in various industries, thus a large amount of FRP wastes have been generated due to the out-of-service of FRP products. Recycling FRP wastes into coarse aggregates to replace natural coarse aggregates (NCA) to form the recycled FRP aggregate concrete (RFAC) is a potential approach to dispose of huge quantities of FRP wastes with low environmental impact. In this paper, waste glass FRP (GFRP) bars were cut into particles of 12 sizes to enable the grading of recycled FRP aggregate (RFA) as similar as possible to that of NAC. The influence of different RFA volume replacement ratios (0%, 30%, 50%, 70%, 100%) on the compressive performance of RFAC was investigated based on uniaxial compression tests of 15 standard cylinders. The results showed that the failure mode of RFAC was different from that of NAC. As the RFA replacement ratio increased, the compressive strength and elastic modulus of the RFAC gradually decreased, but its post-peak brittleness was significantly mitigated compared to NAC. The Poisson's ratio of RFAC increased with the increase in the RGFA replacement ratio at the elastic stage and was smaller than that of NCA concrete. Both the existing stress-strain models developed for NAC and recycled aggregate concrete (RAC) were found not fit for the RFAC. Thus, a new stress-strain model that was applicable to RFAC was developed by modifying the classical existing model, and a good agreement between the model predictions and test data was reached.
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Limestone calcined clay cement (LC3) is successfully used to fabricate engineered cementitious composites (ECC) exhibiting tensile strength σtu of 9.55 ± 0.59 MPa or tensile strain capacity εtu of 8.53 ± 0.30%. The high tensile strength of the composites is closely related to the improvement of fiber/matrix interfacial bond strength, and the high ductility is attributed to the enhancement of fiber dispersion homogeneity. For the case of ECC incorporating 50% LC3, the reduction of initial cracking stress σtc that favors the growth of the crack in a controlled manner also contributes to the improvement of strain hardening behavior. The composition analysis indicates that carboaluminates and additional hydration products including C-(A)-S-H and ettringite are generated, which contributes to the densification of the microstructure of the ECC matrix. The pore structure is thus remarkably refined. Besides, when ordinary Portland cement (OPC) is partly replaced by LC3, the consumed energy and equivalent CO2 emission decrease, especially the equivalent CO2 emission with the reduction ratio attaining 40.31%. It is found that ECC using 35% LC3 exhibits the highest mechanical resistance and ECC incorporating 50% LC3 shows the highest ductility from the environmental point of view.
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To promote the sustainable development of the construction industry, concrete incorporating polyethylene (PE) fiber-strengthened recycled coarse aggregate (SRCA) and seawater and sea sand (SWSS) is prepared. The usage of SRCA significantly improves the mechanical performance of concrete. The strength is improved, and the failure mode of concrete cylinders is also remarkably altered. The incorporation of SWSS that alleviates the shortage of freshwater and river sand slightly reduces the mechanical strength of concrete at 28 and 90 days, while the replacement of cement by 35% limestone calcined clay cement (LC3) overcomes this drawback. The compressive strength of concrete is further enhanced, and the pore structure is refined. The introduction of LC3 also promotes the formation of Friedel's salt, which could improve the chloride binding capacity of concrete using SWSS. Furthermore, the stress-strain relationship of sustainable concrete is analyzed, and the experimental results are compared with the commonly used constitutive models. The predictive constitutive models are proposed to effectively describe the mechanical performance of sustainable concrete.
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The adsorption of bio-polyols from dilute aqueous solution is important but faces challenges in the sustainable bio-refinery process. One solution to increase adsorption efficiency is to leverage host-guest interactions between the polyols and materials to grant a preference for polyols. In this study, we synthesized MIL-53 and diverse OH-bonded variants, and studied their adsorption properties towards ethanediol, 1,3-propanediol and glycerol in water. Among the four materials, OH-MIL-53 exhibited fast adsorption kinetics and high capacity, and could be completely regenerated through ethanol elution. Hydrophobic interactions between the alkyl chains of the polyols and the organic linkers of OH-MIL-53 and hydrogen bonding interactions between their OH groups were identified. The synergistic effect of the host-guest interactions is responsible for the unique adsorption performances of OH-MIL-53 towards polyols, and particularly for 1,3-propanediol.
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In the interest of solving the resource and environmental problems of the construction industry, low-carbon geopolymer coating ensures great durability and extends the service life of existing infrastructure. This paper presents a multidisciplinary assessment of the protective performance and environmental impacts of geopolymer coating. Various parameters, such as main substance, water-solid (W/S) ratio, activator type and curing time, were investigated for their effects on interface characterization in terms of contact angle, surface energy, mechanical properties and microstructure. These parameters had negligible effects on the amounts and types of hydrophilic functional groups of geopolymer surfaces. A combination of organic surface modifiers and geopolymer coatings was shown to ensure hydrophobic surface conditions and great durability. Silicon-based modifiers exhibited better wetting performance than capillary crystalline surfactants by eliminating hydroxyl groups and maintaining structural backbone Si-O-T (Si, Al) on geopolymers' surfaces. Finally, life-cycle analysis was conducted to investigate the environmental performance. Geopolymer coating yielded substantially lower environmental impacts (50-80% lower in most impact categories) than ordinary Portland cement (OPC) coating. Silicon-based modifiers had negligible influence due to their minimal usage. Increasing the W/S ratio diluted the geopolymer coating and decreased the environmental impacts, and slag-based geopolymer coating achieved lower environmental impacts than FA-based and MK-based varietie.
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In response to resource shortage and carbon dioxide emissions, an innovative type of sustainable concrete containing LC3, seawater, sea sand, and surface-treated recycled aggregates is proposed in this study to replace traditional concrete. To understand the bond properties between the sustainable concrete and CFRP bars, an investigation was conducted on the bond behavior between sand-coated CFRP bars and advanced sustainable concrete. Pull-out tests were carried out to reveal the failure mechanisms and performance of this bond behavior. The results showed that the slip increased monotonically along with the increase in confinement. The bond strength increased up to approximately 15 MPa, and the critical ratio of C/D was reached. The critical ratio approached 3.5 for the Portland cement groups, while the ratio was determined as approximately 4.5 when LC3 was introduced. When the proportion of LC3 reached 50%, there was a reduction in bond strength. A multisegmented modified bond-slip model was developed to describe the four-stage bond behavior. In terms of bond strength and slip, the proposed advanced concrete exhibited almost identical bond behavior to other types of concrete.