A nickel oxide nanoflakes/reduced graphene oxide composite and its high-performance lithium-storage properties

Journal of Solid State Electrochemistry - Since conventional graphite-based anode possesses a low capacity, seeking for high-capacity anode candidates becomes significant for constructing emerging...     

Optical vortices in the Ginzburg–Landau equation with cubic–quintic nonlinearity

In a dissipative system with cubic–quintic nonlinearity, the curious evolution of optical vortex beams characterized by different topological charges (TCs) is simulated numerically and presented their evolution profiles. We find that new vortices will be induced during propagation, and the behavior of vortices, as affected by the TC and the number of beads of the incident beam, as well as its size, is also discussed. Common rules associated with the initial conditions coming from various incident beams are developed to determine the number of induced vortices and the corresponding rotation direction. Attributed to the nonlinearity, during propagation we see the beams slowly expand to induce new vortices, which commonly appear in oppositely charged pairs, while the net topological charge of the vortex is conserved. Our results not only deepen the understanding of optical vortices, but also widen their potential applications.     

Diversity-oriented synthesis and antifungal activities of novel pimprinine derivative bearing a 1,3,4-oxadiazole-5-thioether moiety

Molecular Diversity - Based on the strategy of diversity-oriented synthesis and the structures of natural product pimprinine and streptochlorin, two series of novel pimprinine derivatives...     

Bi/Bi_2O_3 nanoparticles supported on N-doped reduced graphene oxide for highly efficient CO_2 electroreduction to formate

Electrocatalytic CO_2 reduction(CO_2 ER) into formate is a desirable route to achieve efficient transformation of CO_2 to value-added chemicals,however,it still suffers from limited catalytic activity and poor selectivity.Herein,we develop a hybrid electrocatalyst composed of bismuth and bismuth oxide nanoparticles(NPs) supported on nitrogen-doped reduced graphene oxide(Bi/Bi_2 O_3/NrGO) nanosheets prepared by a combined hydrothermal with calcination treatment.Thanks to the combination of undercoordinated sites and strong synergistic effect between Bi and Bi_2 O_3,Bi/Bi_2 O_3/NrGO-700 hybrid displays a promoted CO2 ER catalytic performance and selectivity for formate production,as featured by a small onset potential of-0.5 V,a high current density of-18 mA/cm~2,the maximum Faradaic efficiency of85% at-0.9 V,and a low Tafel slope of 166 mV/dec.Experimental results reveal that the higher CO_2 ER performance of Bi/Bi_2 O_3/NrGO-700 than that of Bi NPs supported on NrGO(Bi/NrGO) can be due to the partial reduction of Bi_2 O_3 NPs into Bi,which significantly increases undercoordinated active sites on Bi NPs surface,thus boosting its CO_2 ER performance.Furthermore,a two-electrode device with Ir/C anode and Bi/Bi_2 O_3/NrGO-700 cathode could be integrated with two alkaline batteries or a planar solar cell to achieve highly active water splitting and CO_2 ER.     

The first excited single-proton resonance in 15F by complex-scaled Green's function method

The complex-scaled Green's function(CGF)method is employed to explore the single-proton resonance in 15F.Special attention is paid to the first excited resonant state 5/2+,which has been widely studied in both theory and experiments.However,past studies generally overestimated the width of the 5/2+state.The predicted energy and width of the first excited resonant state 5/2+by the CGF method are both in good agreement with the experimental value and close to Fortune's new estimation.Furthermore,the influence of the potential parameters and quadruple deformation effects on the resonant states are investigated in detail,which is helpful to the study of the shell structure evolution.     

A unified framework for mapping individual interregional high-order morphological connectivity based on regional cortical features from anatomical MRI

Building individual brain networks form the single volume of anatomical MRI is a challenging task. Furthermore, the high-order connectivity of morphological networks remains unexplored. This paper aimed to investigate the individual high-order morphological connectivity from anatomical MRI. Towards this goal, a unified framework based on six feature distances (euclidean, seuclidean, mahalanobis, cityblock, minkowski, and chebychev) was proposed to derive high-order interregional morphological features. The test-retest datasets and the healthy aging datasets were applied to analyze the reliability and the inter-subject variability of the novel features. In addition, the predictive models based on these novel features were established for age estimation. The proposed six neuroanatomical features exhibited significant high-to-excellent reliability. Certain connections were significantly correlated to biological age based on the six novel metrics (p < .05, FDR corrected). Moreover, the predicted age were significantly correlated to the original age in each regression task (r > 0.5, p < 10⁻⁶). The results suggested that the novel high-order metrics were reliable and could reflect individual differences, which could be beneficial for current methods of individual brain connectomes.     

A Triply Negatively Charged Nanographene Bilayer with Spin Frustration

We report on the largest open-shell graphenic bilayer and also the first example of triply negatively charged radical π-dimer. Upon three-electron reduction, bilayer nanographene fragment molecule (C₉₆H₂₄Ar₆)₂ (Ar=2,6-dimethylphenyl) ( 1 ₂) was transformed to a triply negatively charged species 1 ₂^3.−, which has been characterized by single-crystal X-ray diffraction, electron paramagnetic resonance (EPR) spectroscopy and magnetic properties on a superconducting quantum interference device (SQUID). 1 ₂^3.− features a 96-center-3-electron (96c/3e) pancake bond with a doublet ground state, which can be thermally excited to a quartet state. It consists of 34 π-fused rings with 96 conjugated sp² carbon atoms. Spin frustration is observed with the frustration parameter f>31.8 at low temperatures in 1 ₂^3.−, which indicates graphene upon reduction doping may behave as a quantum spin liquid.     

Synthesis of a Porous [14]Annulene Graphene Nanoribbon and a Porous [30]Annulene Graphene Nanosheet on Metal Surfaces

The electrical and mechanical properties of graphene-based materials can be tuned by the introduction of nanopores, which are sensitively related to the size, morphology, density, and location of nanopores. The synthesis of low-dimensional graphene nanostructures containing well-defined nonplanar nanopores has been challenging due to the intrinsic steric hindrance. Herein, we report the selective synthesis of one-dimensional (1D) graphene nanoribbons (GNRs) containing periodic nonplanar [14]annulene pores on Ag(111) and two-dimensional (2D) porous graphene nanosheet containing periodic nonplanar [30]annulene pores on Au(111), starting from a same precursor. The formation of distinct products on the two substrates originates from the different thermodynamics and kinetics of coupling reactions. The reaction mechanisms were confirmed by a series of control experiments, and the appropriate thermodynamic and kinetic parameters for optimizing the reaction pathways were proposed. In addition, the combined scanning tunneling spectroscopy (STS) and density functional theory (DFT) calculations revealed the electronic structures of porous graphene structures, demonstrating the impact of nonplanar pores on the π-conjugation of molecules.     

Single-pulse shock-tube study on the pyrolysis of small esters (ethyl and propyl propanoate,isopropyl acetate) and methyl isopropyl carbonate

Single-pulse shock-tube experiments were used to study the thermal decomposition of selected oxygenated hydrocarbons: Ethyl propanoate (C₂H₅OC(O)C₂H₅; EP), propyl propanoate (C₃H₇OC(O)C₂H₅; PP), isopropyl acetate ((CH₃)₂HCOC(O)CH₃; IPA), and methyl isopropyl carbonate ((CH₃)₂HCOC(O)OCH₃; MIC) The consumption of reactants and the formation of stable products such as C₂H₄ and C₃H₆ were measured with gas chromatography/mass spectrometry (GC/MS). Depending on the considered reactant, the temperatures range from 716–1102 K at pressures between 1.5 and 2.0 bar. Rate-coefficient data were obtained from first-order analysis. All reactants primarily decompose by six-center eliminations: EP → C₂H₄ + C₂H₅COOH (propionic acid); PP → C₃H₆ + C₂H₅COOH; IPA → C₃H₆ + CH₃COOH (acetic acid); MIC → C₃H₆ + CH₃OC(O)OH (methoxy formic acid). Experimental rate-coefficient data can be well represented by the following Arrhenius expressions: k(EP → products) = 10^13.49±0.16 exp(−214.95±3.25 kJ/mol/RT) s⁻¹; k(PP → products) = 10^12.21±0.16 exp(–191.21±2.79 kJ/mol/RT) s⁻¹; k(IPA → products) = 10^13.10±0.31 exp(–186.38±5.10 kJ/mol/RT) s⁻¹; k(MIC → products) = 10^12.43±0.29 exp(–165.25±4.46 kJ/mol/RT) s⁻¹. The determination of rate coefficients was based on the amount of C₂H₄ or C₃H₆ formed. The potential energy surface (PES) of the thermal decomposition of these four reactants was determined with the G4 composite method. A master-equation analysis was conducted based on energies and molecular properties from the G4 computations. The results indicate that the length of a linear alkyl substituent does not significantly influence the rate of six-center eliminations, whereas the change from a linear to a branched alkyl substituent results in a significant reactivity increase. The comparison between rate-coefficient data also shows that alkyl carbonates have higher reactivity towards decomposition by six-center elimination than esters. The results are discussed in in the context of reactivity patterns of carbonyl compounds.     

Theoretical insights into the mechanism of photocatalytic reduction of CO2 over semiconductor catalysts

Photocatalytic reduction of CO₂ is one important approach to alleviate greenhouse gas emission and energy crisis, which has gained huge attention in the past decades. However, the lack of understanding complex reaction mechanism impedes new catalysts design. It is also very difficult to understand the mechanism by using only experimental approaches. For this concern, theoretical calculations can effectively supplement the experimental deficiency and thus play an important role. Recently theoretical calculations have been performed on adsorption, migration and reduction of CO₂ molecule on the photocatalyst surface, leading to useful information that have contributed greatly to this field. This review summarizes recent advances in first-principles calculations about CO₂ photoreduction over various semiconductor photocatalysts like metal oxides, sulfides and g-C₃N₄. The methods, models, adsorption and reaction pathways have been discussed in detail. The perspective about future investigation on the photocatalytic reduction of CO₂ using first principles calculations is also presented.