In comparison with the fast development of binary mixture separations, ternary mixture separations are significantly more difficult and have rarely been realized by a single material. Herein, a new ...strategy of tuning the gate‐opening pressure of flexible MOFs is developed to tackle such a challenge. As demonstrated by a flexible framework NTU‐65, the gate‐opening pressure of ethylene (C2H4), acetylene (C2H2), and carbon dioxide (CO2) can be regulated by temperature. Therefore, efficient sieving separation of this ternary mixture was realized. Under optimized temperature, NTU‐65 adsorbed a large amount of C2H2 and CO2 through gate‐opening and only negligible amount of C2H4. Breakthrough experiments demonstrated that this material can simultaneously capture C2H2 and CO2, yielding polymer‐grade (>99.99 %) C2H4 from single breakthrough separation.
One‐step sieving separation of a ternary gas mixture (C2H2/CO2/C2H4) has been realized by a flexible MOF NTU‐65. Successful separation relies on tuning the gate‐opening pressure of this flexible framework to optimize the separation performance. Under an optimized temperature, NTU‐65 adsorbed large amount of C2H2 and CO2 but a negligible amount of C2H4, readily producing high‐purity C2H4 through a separation column.
Full text
Available for:
BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Literature has indicated that accurate dietary assessment is very important for assessing the effectiveness of weight loss interventions. However, most of the existing dietary assessment methods rely ...on memory. With the help of pervasive mobile devices and rich cloud services, it is now possible to develop new computer-aided food recognition system for accurate dietary assessment. However, enabling this future Internet of Things-based dietary assessment imposes several fundamental challenges on algorithm development and system design. In this paper, we set to address these issues from the following two aspects: (1) to develop novel deep learning-based visual food recognition algorithms to achieve the best-in-class recognition accuracy; (2) to design a food recognition system employing edge computing-based service computing paradigm to overcome some inherent problems of traditional mobile cloud computing paradigm, such as unacceptable system latency and low battery life of mobile devices. We have conducted extensive experiments with real-world data. Our results have shown that the proposed system achieved three objectives: (1) outperforming existing work in terms of food recognition accuracy; (2) reducing response time that is equivalent to the minimum of the existing approaches; and (3) lowering energy consumption which is close to the minimum of the state-of-the-art.
Abstract Purpose Many dietary factors have either proinflammatory or anti-inflammatory properties. We previously developed a dietary inflammatory index (DII) to assess the inflammatory potential of ...diet. In this study, we conducted a construct validation of the DII based on data from a food frequency questionnaire and three inflammatory biomarkers in a subsample of 2567 postmenopausal women in the Women's Health Initiative Observational Study. Methods We used multiple linear and logistic regression models, controlling for potential confounders, to test whether baseline DII predicted concentrations of interleukin-6, high-sensitivity C-reactive protein (hs-CRP), tumor necrosis factor alpha receptor 2, or an overall biomarker score combining all three inflammatory biomarkers. Results The DII was associated with the four biomarkers with beta estimates (95% confidence interval) comparing the highest with lowest DII quintiles as follows: interleukin-6: 1.26 (1.15–1.38), Ptrend < .0001; tumor necrosis factor alpha receptor 2: 81.43 (19.15–143.71), Ptrend = .004; dichotomized hs-CRP (odds ratio for higher vs. lower hs-CRP): 1.30 (0.97–1.67), Ptrend = .34; and the combined inflammatory biomarker score: 0.26 (0.12–0.40), Ptrend = .0001. Conclusions The DII was significantly associated with inflammatory biomarkers. Construct validity of the DII indicates its utility for assessing the inflammatory potential of diet and for expanding its use to include associations with common chronic diseases in future studies.
Full text
Available for:
GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
To perform construct validation of the population-based Dietary Inflammatory Index (DII) using dietary data from two different dietary assessments and serum high-sensitivity C-reactive protein ...(hs-CRP) as the construct validator.
Using data derived from (i) three 24 h dietary recalls (24HR) at baseline and at the end of each subsequent quarter (i.e. up to fifteen over a year) and (ii) a 7 d dietary recall (7DDR) measured at baseline and then quarterly, regression analyses were conducted to test the effect of the DII score on serum hs-CRP as dichotomous (≤3 mg/l, >3 mg/l), while controlling for important potential confounders.
Existing data from the Seasonal Variation of Blood Cholesterol Study (SEASONS), a longitudinal observational study of healthy participants recruited in Worcester, MA, USA and participants were followed for 1 year.
Participants who had at least one hs-CRP measurement over her/his 1-year participation (n 495 for 24HR, n 559 for 7DDR).
Higher DII scores were associated with values of hs-CRP >3 mg/l (OR = 1·08; 95 % CI 1·01, 1·16, P = 0·035 for the 24HR; and OR = 1·10; 95 % CI 1·02, 1·19, P = 0·015 for the 7DDR).
The population-based DII was associated with interval changes in hs-CRP using both the 24HR and 7DDR. The success of this first-of-a-kind attempt at relating individuals' intakes of inflammation-modulating foods using this refined DII, and the finding that there is virtually no drop-off in predictive capability using a structured questionnaire in comparison to the 24HR standard, sets the stage for use of the DII in a wide variety of other epidemiological and clinical studies.
Reaction in well-designed solids allows yielding products with high selectivity and unique compounds that cannot be obtained in solution. However, the precise tuning of the arrangement of reactants ...in solids for the versatile application of solid-phase reactions remains a challenging subject. Here, a 2 + 2 photocyclization reaction at different positions of the carbon–carbon bonds is described in which the spatial arrangement of 4-styrylpyridines (4-spy) is changed by guest molecules in a flexible metal–organic framework. The 4-spy molecules undergo photodimerization between two carbon–carbon double bonds in the guest-free framework, whereas a reaction between olefinic and aromatic carbon–carbon bonds or the absence of reaction takes place in the solvent-incorporated form. This reactivity, which can be termed as “dynamic topochemistry” contributes to enforce the applicability of solid-phase reactions in synthetic chemistry.
Full text
Available for:
IJS, KILJ, NUK, PNG, UL, UM
The structure and activity in CO oxidation of Ag/CeO2 employing CeO2 nanorods and nanocubes as the support have been studied. The experimental results reveal the shape-dependent interplay between ...oxygen vacancies and Ag-CeO2 interaction and their influence on the catalytic activity. Silver supported on CeO2 nanocubes with a loading of 1% shows the highest specific catalytic activity. Display omitted
► The interplay between oxygen vacancies and Ag–CeO2 interaction depends on the shape of CeO2. ► Such an interplay controls the structures and catalytic activity of Ag/CeO2 catalysts. ► CeO2 nanorods stabilize cationic Ag species. ► CeO2 nanocubes facilitate the formation of metallic Ag nanoparticles. ► The Ag nanoparticle–CeO2 interface is the active structure in catalyzing CO oxidation.
Ag/CeO2 catalysts employing CeO2 nanocubes (c-CeO2) and nanorods (r-CeO2) as the support were prepared by conventional incipient wetness impregnation followed by calcination at 500°C in air. Their structures have been characterized in detail and their catalytic activities in CO oxidation have also been tested. c-CeO2 and r-CeO2 nanocrystals exhibit different concentrations and structures of oxygen vacancies. The silver-r-CeO2 interaction is stronger than the silver-c-CeO2 interaction. Fine Ag nanoparticles form in 1%-Ag/c-CeO2 and grow in size in 3%-Ag/c-CeO2; however, positively charged Agn+ clusters dominate in 1%-Ag/r-CeO2, and fine Ag nanoparticles dominate in 3%-Ag/r-CeO2. Supported Ag nanoparticles are much more capable of creating oxygen vacancies in CeO2 than supported positively charged Agn+ clusters. More oxygen vacancies form in Ag/c-CeO2 than in Ag/r-CeO2. The average charge density of oxygen vacancies and the ratio between large oxygen vacancy clusters and small vacancies in CeO2 nanocrystals are enhanced when loaded with positively charged Agn+ clusters but reduced when loaded with Ag nanoparticles. Ag nanoparticles greatly promote the reduction and catalytic activity in CO oxidation of CeO2 nanocrystals but positively charged Agn+ clusters do not. These results demonstrate the concept that the interplay between oxygen vacancies and Ag–CeO2 interaction controls the structures of silver and CeO2 in Ag/CeO2 catalysts and thus their surface reactivity and catalytic activity, deepening the fundamental understanding of metal/CeO2 catalysts. These results also reveal that the interplay between oxygen vacancies and Ag–CeO2 interaction in Ag/CeO2 catalysts depends on the shape of CeO2 support, opening up a new strategy for the design of efficient and economic metal/CeO2 catalysts by engineering the shape of CeO2 support.
Full text
Available for:
GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Pd nanocrystals were prepared by the reduction of a H2PdCl4 aqueous solution with C2H4 in the presence of different amounts of poly(N-vinyl-2-pyrrolidone) (PVP). Their average size decreases ...monotonically as the PVP monomer/Pd molar ratio increases up to 1.0 and then does not vary much at higher PVP monomer/Pd molar ratios. Infrared spectroscopy and X-ray photoelectron spectroscopy results reveal the interesting size-dependent interaction of PVP molecules with Pd nanocrystals. For fine Pd nanocrystals capped with a large number of PVP molecules, each PVP molecule chemisorbs with its oxygen atom in the ring; for large Pd nanocrystals capped by a small number of PVP molecules, each PVP molecule chemisorbs with both the oxygen atom and nitrogen atom in the ring, which obviously affects the structure of chemisorbed PVP molecules and even results in the breaking of involved C–N bonds of some chemisorbed PVP molecules. Charge transfer always occurs from a chemisorbed PVP ligand to Pd nanocrystals. These results provide novel insights into the PVP–metal nanocrystal interaction, which are of great importance in the fundamental understanding of surface-mediated properties of PVP-capped metal nanocrystals.
Full text
Available for:
IJS, KILJ, NUK, PNG, UL, UM
•Au supported on various carbon materials (RGO, AC and GC) has been prepared.•The catalytic activities were tested in the aerobic oxidation of benzyl alcohol.•Au/RGO shows superior activity compared ...to Au/AC and Au/GC.•The effect of the nature of carbon supports is discussed.
Various Au/C catalysts were prepared by Au nanoparticels supported on different carbonaceous supports including reduced graphene oxide (RGO), activated carbon (AC) and graphite (GC) using sol-immobilization method. Au/RGO shows a much higher activity than Au/AC and Au/GC in the liquid phase aerobic oxidation of benzyl alcohol. The superior catalytic performance of Au/RGO may be related to the presence of surface O-containing functional groups and moderate graphite character of RGO supports.
Full text
Available for:
GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
The interaction of atomic hydrogen and H2O with stoichiometric and partially reduced CeO2(111) thin films deposited on a Cu(111) substrate was investigated by temperature programmed desorption and ...X-ray photoelectron spectroscopy. On stoichiometric CeO2(111) surface, the adsorption of atomic H(g) leads to the formation of surface hydroxyl (OH(a)) and H2O(a) as well as the reduction of Ce4+ into Ce3+. On reduced CeO2(111) surfaces, the stability of OH(a) was enhanced by the presence of oxygen vacancies. Upon heating, surface hydroxyls undergo two competing reaction pathways: one is the associative desorption of OH(a) releasing H2O and creating oxygen vacancies (OH(a) + OH(a) → H2O(g) + Olattice + Ovacancy), and the other one is to produce H2 via OH(a) + OH(a) → H2(g) + 2Olattice. The presence of oxygen vacancies in CeO2 favors the reaction pathway of H2 formation. At 115 K, reversible dissociation and molecular adsorption of H2O occur on stoichiometric CeO2(111) surface, but irreversible dissociation of H2O occurs on reduced CeO2(111) surfaces. These results deepen the fundamental understanding of the influence of oxygen vacancies on the reactivity of surface hydroxyls and water on CeO2 surface.
Full text
Available for:
IJS, KILJ, NUK, PNG, UL, UM
Background
Various dietary components have been studied in relation to overall mortality; however, little is known about the relationship between the inflammatory potential of overall diet and ...mortality.
Materials and methods
We examined the association between the dietary inflammatory index (DII) and mortality in the National Health and Nutrition Examination Survey III follow-up study. The DII was computed from baseline dietary intake assessed using 24-h dietary recalls (1988–1994). Mortality was determined from the National Death Index records through 2006. Cox proportional hazards regression was used to estimate hazard ratios (HRs) and 95 % confidence interval (95 % CI). During the follow-up, 2795 deaths were identified, including 1233 due to cardiovascular disease (CVD), and 615 due to cancer, 158 of which were due to digestive-tract cancers.
Results
Multivariate Cox proportional hazards regression analyses, adjusting for age, race, diabetes status, hypertension, physical activity, body mass index, poverty index, and smoking, revealed positive associations between higher DII scores and mortality. Comparing subjects in DII tertile 3 versus tertile 1, significant associations were noted for all-cause mortality (HR
Tertile3vs1
1.34; 95 % CI 1.19–1.51,
P
trend
< 0.0001), CVD mortality (HR
Tertile3vs1
1.46; 95 % CI 1.18–1.81,
P
trend
= 0.0006), cancer mortality (HR
Tertile3vs1
1.46; 95 % CI 1.10–1.96,
P
trend
= 0.01), and digestive-tract cancer mortality (HR
Tertile3vs1
2.10; 95 % CI 1.15–3.84,
P
trend
= 0.03).
Conclusion
These results indicate that a pro-inflammatory diet, as indicated by higher DII scores, was associated with higher risk of all-cause, CVD, and cancer mortality.
Full text
Available for:
DOBA, EMUNI, FIS, FSPLJ, FZAB, GEOZS, GIS, IJS, IMTLJ, IZUM, KILJ, KISLJ, MFDPS, NLZOH, NUK, OBVAL, OILJ, PILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, SIK, UILJ, UKNU, UL, UM, UPUK, VKSCE, VSZLJ, ZAGLJ
PDF
