34 research outputs found

    Tuning Open Metal Site-Free <b>ncb</b> Type of Metal–Organic Frameworks for Simultaneously High Gravimetric and Volumetric Methane Storage Working Capacities

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    The design and synthesis of a single metal–organic framework (MOF) material with simultaneously high gravimetric and volumetric methane storage working capacities are still a great challenge. The open metal site (OMS) in MOFs is generally regarded as an advantage to enhance host–guest affinity. However, it is detrimental to the methane storage working capacity to some extent due to the resulting high low-pressure uptake. Moreover, the reported methane storage MOFs are predominately focusing on edge-transitive or low-connected mixed-linker networks. In contrast, high-connected mixed-linker MOFs have been less investigated for methane storage. Herein, three isoreticular nine-connected trinuclear iron-based Fe-ncb-MOFs without OMSs have been judiciously designed and successfully constructed by means of the mixed-linker approach associated with the fixing amide-functionalized pyridyl-carboxylate ligand LP (4-(pyridin-4-ylcarbamoyl)­benzoate) and three differing sized dicarboxylate ligands. High-pressure methane adsorption measurements show that, with the isoreticular extension from BDC (1,4-benzenedicarboxylate) to BPDC (4,4′-biphenyldicarboxylate) and ABDC (azobenzene-4,4′-dicarboxylate), three Fe-ncb-MOFs exhibit gradually increasing not only gravimetric but also volumetric storage capacities because of their balancing gravimetric surface area and volumetric surface area, hierarchical pore system, and modest CH4 heats of adsorption. Among them, the Fe-ncb-ABDC demonstrates a rare combination of simultaneously high gravimetric and volumetric CH4 storage working capacities of 0.302/0.37 g g–1 and 196/240 cm3 (STP) cm–3 at 298/273 K and between 80 and 5 bar, respectively, which outperform the 8-c Fe-8T18-ABDC assembled from a shorter pyridyl-carboxylate ligand IN (isonicotinate) and ABDC, due to its limited pore volume, the presence of OMSs, and more confined pore spaces, and place Fe-ncb-ABDC among the best performing MOFs

    Tuning Open Metal Site-Free <b>ncb</b> Type of Metal–Organic Frameworks for Simultaneously High Gravimetric and Volumetric Methane Storage Working Capacities

    No full text
    The design and synthesis of a single metal–organic framework (MOF) material with simultaneously high gravimetric and volumetric methane storage working capacities are still a great challenge. The open metal site (OMS) in MOFs is generally regarded as an advantage to enhance host–guest affinity. However, it is detrimental to the methane storage working capacity to some extent due to the resulting high low-pressure uptake. Moreover, the reported methane storage MOFs are predominately focusing on edge-transitive or low-connected mixed-linker networks. In contrast, high-connected mixed-linker MOFs have been less investigated for methane storage. Herein, three isoreticular nine-connected trinuclear iron-based Fe-ncb-MOFs without OMSs have been judiciously designed and successfully constructed by means of the mixed-linker approach associated with the fixing amide-functionalized pyridyl-carboxylate ligand LP (4-(pyridin-4-ylcarbamoyl)­benzoate) and three differing sized dicarboxylate ligands. High-pressure methane adsorption measurements show that, with the isoreticular extension from BDC (1,4-benzenedicarboxylate) to BPDC (4,4′-biphenyldicarboxylate) and ABDC (azobenzene-4,4′-dicarboxylate), three Fe-ncb-MOFs exhibit gradually increasing not only gravimetric but also volumetric storage capacities because of their balancing gravimetric surface area and volumetric surface area, hierarchical pore system, and modest CH4 heats of adsorption. Among them, the Fe-ncb-ABDC demonstrates a rare combination of simultaneously high gravimetric and volumetric CH4 storage working capacities of 0.302/0.37 g g–1 and 196/240 cm3 (STP) cm–3 at 298/273 K and between 80 and 5 bar, respectively, which outperform the 8-c Fe-8T18-ABDC assembled from a shorter pyridyl-carboxylate ligand IN (isonicotinate) and ABDC, due to its limited pore volume, the presence of OMSs, and more confined pore spaces, and place Fe-ncb-ABDC among the best performing MOFs

    Tuning Open Metal Site-Free <b>ncb</b> Type of Metal–Organic Frameworks for Simultaneously High Gravimetric and Volumetric Methane Storage Working Capacities

    No full text
    The design and synthesis of a single metal–organic framework (MOF) material with simultaneously high gravimetric and volumetric methane storage working capacities are still a great challenge. The open metal site (OMS) in MOFs is generally regarded as an advantage to enhance host–guest affinity. However, it is detrimental to the methane storage working capacity to some extent due to the resulting high low-pressure uptake. Moreover, the reported methane storage MOFs are predominately focusing on edge-transitive or low-connected mixed-linker networks. In contrast, high-connected mixed-linker MOFs have been less investigated for methane storage. Herein, three isoreticular nine-connected trinuclear iron-based Fe-ncb-MOFs without OMSs have been judiciously designed and successfully constructed by means of the mixed-linker approach associated with the fixing amide-functionalized pyridyl-carboxylate ligand LP (4-(pyridin-4-ylcarbamoyl)­benzoate) and three differing sized dicarboxylate ligands. High-pressure methane adsorption measurements show that, with the isoreticular extension from BDC (1,4-benzenedicarboxylate) to BPDC (4,4′-biphenyldicarboxylate) and ABDC (azobenzene-4,4′-dicarboxylate), three Fe-ncb-MOFs exhibit gradually increasing not only gravimetric but also volumetric storage capacities because of their balancing gravimetric surface area and volumetric surface area, hierarchical pore system, and modest CH4 heats of adsorption. Among them, the Fe-ncb-ABDC demonstrates a rare combination of simultaneously high gravimetric and volumetric CH4 storage working capacities of 0.302/0.37 g g–1 and 196/240 cm3 (STP) cm–3 at 298/273 K and between 80 and 5 bar, respectively, which outperform the 8-c Fe-8T18-ABDC assembled from a shorter pyridyl-carboxylate ligand IN (isonicotinate) and ABDC, due to its limited pore volume, the presence of OMSs, and more confined pore spaces, and place Fe-ncb-ABDC among the best performing MOFs

    Tuning Open Metal Site-Free <b>ncb</b> Type of Metal–Organic Frameworks for Simultaneously High Gravimetric and Volumetric Methane Storage Working Capacities

    No full text
    The design and synthesis of a single metal–organic framework (MOF) material with simultaneously high gravimetric and volumetric methane storage working capacities are still a great challenge. The open metal site (OMS) in MOFs is generally regarded as an advantage to enhance host–guest affinity. However, it is detrimental to the methane storage working capacity to some extent due to the resulting high low-pressure uptake. Moreover, the reported methane storage MOFs are predominately focusing on edge-transitive or low-connected mixed-linker networks. In contrast, high-connected mixed-linker MOFs have been less investigated for methane storage. Herein, three isoreticular nine-connected trinuclear iron-based Fe-ncb-MOFs without OMSs have been judiciously designed and successfully constructed by means of the mixed-linker approach associated with the fixing amide-functionalized pyridyl-carboxylate ligand LP (4-(pyridin-4-ylcarbamoyl)­benzoate) and three differing sized dicarboxylate ligands. High-pressure methane adsorption measurements show that, with the isoreticular extension from BDC (1,4-benzenedicarboxylate) to BPDC (4,4′-biphenyldicarboxylate) and ABDC (azobenzene-4,4′-dicarboxylate), three Fe-ncb-MOFs exhibit gradually increasing not only gravimetric but also volumetric storage capacities because of their balancing gravimetric surface area and volumetric surface area, hierarchical pore system, and modest CH4 heats of adsorption. Among them, the Fe-ncb-ABDC demonstrates a rare combination of simultaneously high gravimetric and volumetric CH4 storage working capacities of 0.302/0.37 g g–1 and 196/240 cm3 (STP) cm–3 at 298/273 K and between 80 and 5 bar, respectively, which outperform the 8-c Fe-8T18-ABDC assembled from a shorter pyridyl-carboxylate ligand IN (isonicotinate) and ABDC, due to its limited pore volume, the presence of OMSs, and more confined pore spaces, and place Fe-ncb-ABDC among the best performing MOFs

    Polynuclear Rare-Earth Cluster-Directed Self-Assembly of Highly Porous Zeolite-like Metal–Organic Frameworks with Methane Storage Property

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    Due to their intrinsic structural features, the design and synthesis of a new type of zeolite-like metal–organic frameworks (ZMOFs) is highly desirable but challenging. Herein, solvothermal reactions between an angular dicarboxylate linker and rare-earth (RE) ions afforded two RE-MOFs, namely, Tb-ZMOF-2 and Tb-ZMOF-3, respectively. Structural analyses reveal that Tb-ZMOF-2 encompasses a novel [446482] cage, while Tb-ZMOF-3 contains nonanuclear (i.e., D6R) and hexanuclear (i.e., D4R) RE clusters simultaneously, subsequently resulting in two new zeolitic topologies. Thanks to its high surface area and pore volume, Tb-ZMOF-2 demonstrates considerably high gravimetric and volumetric methane storage working capacities

    Tuning Open Metal Site-Free <b>ncb</b> Type of Metal–Organic Frameworks for Simultaneously High Gravimetric and Volumetric Methane Storage Working Capacities

    No full text
    The design and synthesis of a single metal–organic framework (MOF) material with simultaneously high gravimetric and volumetric methane storage working capacities are still a great challenge. The open metal site (OMS) in MOFs is generally regarded as an advantage to enhance host–guest affinity. However, it is detrimental to the methane storage working capacity to some extent due to the resulting high low-pressure uptake. Moreover, the reported methane storage MOFs are predominately focusing on edge-transitive or low-connected mixed-linker networks. In contrast, high-connected mixed-linker MOFs have been less investigated for methane storage. Herein, three isoreticular nine-connected trinuclear iron-based Fe-ncb-MOFs without OMSs have been judiciously designed and successfully constructed by means of the mixed-linker approach associated with the fixing amide-functionalized pyridyl-carboxylate ligand LP (4-(pyridin-4-ylcarbamoyl)­benzoate) and three differing sized dicarboxylate ligands. High-pressure methane adsorption measurements show that, with the isoreticular extension from BDC (1,4-benzenedicarboxylate) to BPDC (4,4′-biphenyldicarboxylate) and ABDC (azobenzene-4,4′-dicarboxylate), three Fe-ncb-MOFs exhibit gradually increasing not only gravimetric but also volumetric storage capacities because of their balancing gravimetric surface area and volumetric surface area, hierarchical pore system, and modest CH4 heats of adsorption. Among them, the Fe-ncb-ABDC demonstrates a rare combination of simultaneously high gravimetric and volumetric CH4 storage working capacities of 0.302/0.37 g g–1 and 196/240 cm3 (STP) cm–3 at 298/273 K and between 80 and 5 bar, respectively, which outperform the 8-c Fe-8T18-ABDC assembled from a shorter pyridyl-carboxylate ligand IN (isonicotinate) and ABDC, due to its limited pore volume, the presence of OMSs, and more confined pore spaces, and place Fe-ncb-ABDC among the best performing MOFs

    A Quinary Metal–Organic Framework Composed of One Metal and One Linker with Ethane-Selective Property

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    Solvothermal reaction between Fe3O(CH3COO)6(H2O)3 and terphenyl-3,3′’,5,5′’-tetracarboxylic acid (H4TPTC) afforded a scarce multinary MOF of Quin-Fe-TPTC (Quin and TPTC are abbreviated from quinary and terphenyl-3,3′’,5,5′’-tetracarboxylate, respectively), which exemplifies the first quinary MOF comprising one metal and one linker in contrast to the documented ones assembled from one metal and four linkers or two metals and three linkers. The variation of linker aspect ratio and the deformation of the trinuclear iron cluster may be responsible for creating such a compound. Quin-Fe-TPTC exhibits bihelical channels interconnected through (hemi) cage cavities replete with methyl groups, resulting in C2H6-selective adsorption from a binary C2H6 and C2H4 mixture and benefiting one-step C2H4 purification. This was validated by not only IAST prediction but also by dynamic column breakthrough experiments

    Data_Sheet_1_Antimicrobial Metabolites Produced by Penicillium mallochii CCH01 Isolated From the Gut of Ectropis oblique, Cultivated in the Presence of a Histone Deacetylase Inhibitor.pdf

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    Three chemical epigenetic modifiers [5-azacytidine, nicotinamide, and suberoylanilide hydroxamic acid (SAHA)] were applied to induce the metabolites of Penicillium mallochii CCH01, a fungus isolated from the gut of Ectropis oblique. Metabolite profiles of P. mallochii CCH01 were obviously changed by SAHA treatment. Four metabolites (1–4), including two new natural sclerotioramine derivatives, isochromophilone XIV (1) and isochromophilone XV (2), and two known compounds, sclerotioramine (3) and (+)-sclerotiorin (4), were isolated and purified from P. mallochii CCH01 treated with SAHA. Their structures were determined by spectroscopic analyzes. Anti-phytopathogenic activities of the isolated compounds 1–4 were investigated under laboratory conditions, and compound 4 showed broad and important inhibition activities against Curvularia lunata (IC50 = 2.1 μg/mL), Curvularia clavata (IC50 = 21.0 μg/mL), Fusarium oxysporum f. sp. Mornordica (IC50 = 40.4 μg/mL), and Botryosphaeria dothidea (IC50 = 27.8 μg/mL), which were comparable to those of referenced cycloheximide, with IC50 values of 0.3, 5.0, 12.4, and 15.3 μg/mL, respectively. Ingredients 2 and 3 showed selective and potent activities against Colletotrichum graminicola with IC50 values of 29.9 and 9.7 μg/mL, respectively. Furthermore, the antibacterial bioassays showed that compounds 3 and 4 exhibited strong inhibition activities against Bacillus subtilis, with disc diameters of zone of inhibition (ZOI) of 9.1 mm for both compounds, which were a bit weaker than that of referenced gentamycin with a ZOI of 10.8 mm. Additionally, the new metabolite 1 showed a promising activity against Candida albicans (ZOI = 10.5 mm), comparable to that of positive amphotericin B with a ZOI of 23.2 mm. The present results suggest that chemical epigenetic modifier induction was a promising approach to obtaining antimicrobial metabolites encoded by silent biosynthetic genes of P. mallochii.</p

    Table_1_Recursive Partitioning Analysis of Fractional Low-Frequency Fluctuations in Narcolepsy With Cataplexy.DOC

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    Objective: To identify narcolepsy related regional brain activity alterations compared with matched healthy controls. To determine whether these changes can be used to distinguish narcolepsy from healthy controls by recursive partitioning analysis (RPA) and receiver operating characteristic (ROC) curve analysis.Method: Fifty-one narcolepsy with cataplexy patients (26 adults and 25 juveniles) and sixty matched heathy controls (30 adults and 30 juveniles) were recruited. All subjects underwent a resting-state functional magnetic resonance imaging scan. Fractional low-frequency fluctuations (fALFF) was used to investigate narcolepsy induced regional brain activity alterations among adult and juveniles, respectively. Recursive partitioning analysis and Receiver operating curve analysis was used to seek the ability of fALFF values within brain regions in distinguishing narcolepsy from healthy controls.Results: Compared with healthy controls, both adult and juvenile narcolepsy had lower fALFF values in bilateral medial superior frontal gyrus, bilateral inferior parietal lobule and supra-marginal gyrus. Compared with healthy controls, both adult and juvenile narcolepsy had higher fALFF values in bilateral sensorimotor cortex and middle temporal gyrus. Also juvenile narcolepsy had higher fALFF in right putamen and right thalamus compared with healthy controls. Based on RPA and ROC curve analysis, in adult participants, fALFF differences in right medial superior frontal gyrus can discriminate narcolepsy from healthy controls with high degree of sensitivity (100%) and specificity (88.9%). In juvenile participants, fALFF differences in left superior frontal gyrus can discriminate narcolepsy from healthy controls with moderate degree of sensitivity (57.1%) and specificity (88.9%).Conclusion: Compared with healthy controls, both the adult and juvenile narcolepsy showed overlap brain regions in fALFF differences after case-control comparison. Furthermore, we propose that fALFF value can be a helpful imaging biomarker in distinguishing narcolepsy from healthy controls among both adults and juveniles.</p
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