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| 2. |
- Chen, Zhen, et al.
(författare)
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Design, Synthesis, and Evaluation of Reversible and Irreversible Monoacylglycerol Lipase Positron Emission Tomography (PET) Tracers Using a "Tail Switching" Strategy on a Piperazinyl Azetidine Skeleton
- 2019
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Ingår i: Journal of Medicinal Chemistry. - : American Chemical Society (ACS). - 0022-2623 .- 1520-4804. ; 62:7, s. 3336-3353
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Tidskriftsartikel (refereegranskat)abstract
- Monoacylglycerol lipase (MAGL) is a senile hydrolase that degrades 2-arachidonoylglycerol (2-AG) in the endocannabinoid system (eCB). Selective inhibition of MAGL has emerged as a potential therapeutic approach for the treatment of diverse pathological conditions, including chronic pain, inflammation, cancer, and neurodegeneration. Herein, we disclose a novel array of reversible and irreversible MAGL inhibitors by means of "tail switching" on a piperazinyl azetidine scaffold. We developed a lead irreversible-binding MAGL inhibitor 8 and reversible-binding compounds 17 and 37, which are amenable for radiolabeling with C-11 or F-18. [C-11]8 ([C-11]MAGL-2-11) exhibited high brain uptake and excellent binding specificity in the brain toward MAGL. Reversible radioligands [C-11]17 ([C-11]PAD) and [F-18]37 ([F-18]MAGL-4-11) also demonstrated excellent in vivo binding specificity toward MAGL in peripheral organs. This work may pave the way for the development of MAGL-targeted positron emission tomography tracers with tunability in reversible and irreversible binding mechanisms.
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| 3. |
- Zhang, Wei, et al.
(författare)
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Effect of post-thermal annealing on the performance and charge photogeneration dynamics of PffBT4T-2OD/PC71BM solar cells
- 2019
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Ingår i: Polymers. - : MDPI AG. - 2073-4360. ; 11:3
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Tidskriftsartikel (refereegranskat)abstract
- In this work, we studied influence of post thermal annealing on the performance and charge photogeneration processes of PffBT4T-2OD/PC 71 BM solar cells. As-prepared device exhibits a high-power conversion efficiency of 9.5%, much higher than that after thermal annealing. To understand this phenomenon, we studied charge photogeneration processes in these solar cells by means of time resolved spectroscopy. We associate the degradation of solar cell performance with the reduction of exciton dissociation efficiency and with increased bimolecular recombination of photogenerated charges as a result of annealing. We correlate the generation of localized PffBT4T-2OD polarons observed via spectro-electrochemical measurements with enhancement of the bimolecular charge recombination of annealed solar cells.
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| 4. |
- Akiyama, Kazunori, et al.
(författare)
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First M87 Event Horizon Telescope Results. V. Physical Origin of the Asymmetric Ring
- 2019
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Ingår i: Astrophysical Journal Letters. - : American Astronomical Society. - 2041-8213 .- 2041-8205. ; 875:1
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Tidskriftsartikel (refereegranskat)abstract
- The Event Horizon Telescope (EHT) has mapped the central compact radio source of the elliptical galaxy M87 at 1.3 mm with unprecedented angular resolution. Here we consider the physical implications of the asymmetric ring seen in the 2017 EHT data. To this end, we construct a large library of models based on general relativistic magnetohydrodynamic (GRMHD) simulations and synthetic images produced by general relativistic ray tracing. We compare the observed visibilities with this library and confirm that the asymmetric ring is consistent with earlier predictions of strong gravitational lensing of synchrotron emission from a hot plasma orbiting near the black hole event horizon. The ring radius and ring asymmetry depend on black hole mass and spin, respectively, and both are therefore expected to be stable when observed in future EHT campaigns. Overall, the observed image is consistent with expectations for the shadow of a spinning Kerr black hole as predicted by general relativity. If the black hole spin and M87's large scale jet are aligned, then the black hole spin vector is pointed away from Earth. Models in our library of non-spinning black holes are inconsistent with the observations as they do not produce sufficiently powerful jets. At the same time, in those models that produce a sufficiently powerful jet, the latter is powered by extraction of black hole spin energy through mechanisms akin to the Blandford-Znajek process. We briefly consider alternatives to a black hole for the central compact object. Analysis of existing EHT polarization data and data taken simultaneously at other wavelengths will soon enable new tests of the GRMHD models, as will future EHT campaigns at 230 and 345 GHz.
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| 5. |
- Ma, Yong, et al.
(författare)
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Identification of Four C-40 Isomers by Means of a Theoretical XPS/ NEXAFS Spectra Study
- 2018
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Ingår i: Journal of Physical Chemistry A. - : AMER CHEMICAL SOC. - 1089-5639 .- 1520-5215. ; 122:20, s. 4750-4755
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Tidskriftsartikel (refereegranskat)abstract
- XPS and NEXAFS spectra of four stable C-40 isomers [29(C-2), 31 (C-s), 38(D-2), and 39(D-sd)] have been investigated theoretically. We combined density functional theory and the full core hole potential method to simulate C 1s XPS and NEXAFS spectra for nonequivalent carbon atoms of four stable C-40 fullerene isomers. The NEXAFS showed obvious dependence on the four C-40 isomers, and XPS spectra are distinct for all four isomers, which can be employed to identify the four stable structures of C-40. Furthermore, the individual components of the spectra according to different categories have been investigated, and the relationship between the spectra and the local structures of C atoms was also explored.
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| 6. |
- Su, Xiao-Jun, et al.
(författare)
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Electrocatalytic Water Oxidation by a Dinuclear Copper Complex in a Neutral Aqueous Solution
- 2015
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Ingår i: Angewandte Chemie International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 54:16, s. 4909-4914
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Tidskriftsartikel (refereegranskat)abstract
- Electrocatalytic water oxidation using the oxidatively robust 2,7-[bis(2-pyridylmethyl)aminomethyl]-1,8-naphthyridine ligand (BPMAN)-based dinuclear copper(II) complex, [Cu-2(BPMAN)(-OH)](3+), has been investigated. This catalyst exhibits high reactivity and stability towards water oxidation in neutral aqueous solutions. DFT calculations suggest that the OO bond formation takes place by an intramolecular direct coupling mechanism rather than by a nucleophilic attack of water on the high-oxidation-state (CuO)-O-IV moiety.
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| 7. |
- Zhang, Jun-Rong, et al.
(författare)
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Accurate K-edge X-ray photoelectron and absorption spectra of g-C3N4 nanosheets by first-principles simulations and reinterpretations
- 2019
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Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : ROYAL SOC CHEMISTRY. - 1463-9076 .- 1463-9084. ; 21:41, s. 22819-22830
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Tidskriftsartikel (refereegranskat)abstract
- We performed a density functional theory (DFT) study on X-ray photoelectron (XPS) and absorption (XAS) spectra of graphitic carbon nitride (g-C3N4) nanosheets at the N and C K-edges. A combined cluster-periodic approach was employed to calculate XPS spectra, in which the core ionic potential (IP) of the solid 2D material was computed by subtracting the work function (obtained with periodic conditions) from the gas phase IP (obtained with large cluster models). With amino-terminated supermolecules of different sizes, we obtained convergent spectra and provide new assignments for 5 nitrogen [1 sp(2); 4 sp(3) (bridging, tertiary, and primary/secondary amino nitrogens)] and 4 carbon (all bonded with three nitrogens) local structures. A good agreement with experiments was obtained, with the N1s (C1s) main peak position differing by 0.1-0.2 eV (0.5-0.8 eV). Our simulations show that N1s XPS of pure g-C3N4 contains only two major features at 398.6 and 401.2 eV, contributed from sp(2)-N and sp(3)-N, respectively. The chemical shifts of all sp(3)-N are so close (deviating by 0.3-0.6 eV) that terminal amino groups -NHx (x = 1, 2) will only be distinguished in high-resolution measurements. In C1s XPS, all carbons show similar (deviation < 0.2 eV) IPs, as determined by the same nearest neighbors. We further excluded the effect of shake-up satellites that may change our XPS interpretations by equivalent core hole time-dependent DFT (ECH-TDDFT) simulations. The effect of vibronic coupling is small (redistribution is only 0.1-0.3 eV to the higher-energy region) in the N1s edge as estimated from the asymmetric main peak shape, and negligible in the C1s edge. Quicker size convergence was found in XAS than XPS. In N1s XAS, we identified a weak pi* spectral feature at 400-401 eV for both -NHx and tertiary nitrogens. Our study provides a clear theoretical reference for X-ray spectral fingerprints of different local structures, which is useful for analysis of g-C3N4 based materials with various designed or unavoidable structural modifications. We also highlight our combined cluster-periodic approach in calculating the K-edge XPS spectra of general 2D materials which predicts accurate absolute values.
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| 8. |
- Zhu, Wei, et al.
(författare)
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Molecular insights on the microstructures of nanoconfined glycerol and its aqueous solutions : The effects of interfacial properties, temperature, and glycerol concentration
- 2019
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Ingår i: Journal of Molecular Liquids. - : Elsevier. - 0167-7322 .- 1873-3166. ; 291
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Tidskriftsartikel (refereegranskat)abstract
- In this work, we conducted molecular dynamics simulations to investigate the effects of rutile–liquid and graphene–liquid interfacial properties, glycerol concentrations (i.e., 10%, 40%, 70%, and 100% molar contents), and temperature (i.e., 180, 273, and 320 K) on the microstructures of nanoconfined glycerol and its aqueous solutions. Results indicated that the effect of interfacial properties on the spatial and orientation distributions of nanoconfined glycerol and water molecules was more prominent than that of temperature. In glycerol aqueous solutions, water and glycerol molecules localized into two distinct layers on the hydrophilic rutile surface but partially mixed with each other near the hydrophobic graphene surface, because water molecules near the hydrophobic surface exhibited more random orientations and formed more hydrogen bonds with glycerol molecules than those near the hydrophilic surface. Moreover, interface introduction and increased temperature drastically reduced the hydrogen bonding ability of water molecules in glycerol aqueous solutions. The addition of glycerol molecules can break hydrogen bonds between water molecules and inhibit water crystallization in glycerol aqueous solutions. Temperature and glycerol concentration exerted limited effects on the hydrogen bonding ability of water molecules on hydrophilic surfaces in glycerol aqueous solutions. Meanwhile, the presence of a hydrophilic surface can effectively decelerate hydrogen bond breakage induced by increasing temperature or by decreasing glycerol contents
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