High-Efficiency Oxygen Reduction to Hydrogen Peroxide Catalyzed by Nickel Single-Atom Catalysts with Tetradentate N2O2 Coordination in a Three-Phase Flow Cell

Carbon-supported Ni^II single-atom catalysts with a tetradentate Ni-N₂O₂ coordination formed by a Schiff base ligand-mediated pyrolysis strategy are presented. A Ni^II complex of the Schiff base ligand (R,R)-(−)-N,N′-bis(3,5-di-tert-butylsalicylidene)-1,2-cyclohexanediamine was adsorbed onto a carbon black support, followed by pyrolysis of the modified carbon material at 300 °C in Ar. The Ni-N₂O₂/C catalyst showed excellent performance for the electrocatalytic reduction of O₂ to H₂O₂ through a two-electron transfer process in alkaline conditions, with a H₂O₂ selectivity of 96 %. At a current density of 70 mA cm⁻², a H₂O₂ production rate of 5.9 mol g_cat.⁻¹ h⁻¹ was achieved using a three-phase flow cell, with good catalyst stability maintained over 8 h of testing. The Ni-N₂O₂/C catalyst could electrocatalytically reduce O₂ in air to H₂O₂ at a high current density, still affording a high H₂O₂ selectivity (>90 %). A precise Ni-N₂O₂ coordination was key to the performance.     

A resonance light-scattering (RLS) serving for various quantitative events since 1995: A comment proposed towards how to apprehend well the meaning of RLS and its corresponding guiding role

A resonance light-scattering (RLS), which was creatively suggested for the first time by Pasternack et al. in 1993 [R.F. Pasternack, C. Bustamante, P.J. Collings, A. Giannetto, E.J. Gibbs, J. Am. Chem. Soc. 115 (1993) 5393], have been enjoyably practiced by numerous investigators for various quantitative events since 1995, and hitherto many research papers and some review papers have got published on lots of international journals specialized in or related to analytical and/or bioanalytical sciences. As revealed from these published papers of interests, however, it is a pity that the meaning of RLS is often apprehended unsatisfactorily both in theory and in practice. In this comment, as a result, I would like to do my best to propose an apprehension of the meaning of RLS as full and exact as possible and simultaneously I would like to deliver the important guiding role of this proposed apprehension in the course of the applications of RLS for various quantitative purposes.     

Surface-enhanced Raman scattering of 4,4′-bipyridine on silver by density functional theory calculations

Surface-enhanced Raman scattering (SERS) of 4,4′-bipyridine (BPy) on silver foil substrate was measured using the 488, 514.5, and 1064 nm excitation lines. Density functional theory (DFT) methods were used to calculate the structure and vibrational spectra of Ag–BPy, Ag₃–BPy and Ag₄–BPy complexes with B3LYP/6-31++G(d,p)(C,H,N)/Lanl2dz(Ag) basis set. The Raman bands of BPy were assigned on the basis of the calculation of potential energy distribution. The calculated spectra of Ag–BPy and Ag₄–BPy complexes were much closer to the experimental results of BPy adsorbed on silver surface than that of Ag₃–BPy complexes. The vibrational frequencies that are sensitive to the planar or non-planar structure of BPy and to the dihedral angle of two pyridyl rings were discussed. The DFT results showed that the angles between two pyridyl rings for Ag–BPy and Ag₄–BPy were skewed by about 38.44° and 37.1°, respectively. The energy gaps of the HOMO and LUMO from DFT were 415–912 nm for BPy–Ag complexes. The relative intensities of SERS bands changed with different excitation laser lines. Thus, a chemical enhancement mechanism should play an important role in the SERS of BPy on silver substrate.     

A new car-following model with consideration of inter-vehicle communication

In this paper, we construct a new car-following model with inter-vehicle communication (IVC) to study the driving behavior under an accident. The numerical results show that the proposed model can qualitatively describe the effects of IVC on each vehicle’s speed, acceleration, movement trail, and headway under an accident and that the new model can overcome the full velocity difference (FVD) model’s shortcoming that collisions occur under an accident, which illustrates that the new model can better describe the driving behavior under an accident than the FVD model.     

Continuous detrended cross-correlation analysis on generalized Weierstrass function

The paper mainly introduces a continuous detrended cross-correlation analysis method to detect the long-range fractal scaling behaviors of continuous and integrable functions. The effects of such method are tested by the generalized Weierstrass function with various seeds. It presents accurate scaling characterization as desired by comparing with that from the popular detrended cross-correlation analysis method of discrete case.     

Simple optimized Brenner potential for thermodynamic properties of diamond

We have examined the commonly used Brenner potentials in the context of the thermodynamic properties of diamond. A simple optimized Brenner potential is proposed that provides very good predictions of the thermodynamic properties of diamond. It is shown that, compared to the experimental data, the lattice wave theory of molecular dynamics (LWT) with this optimized Brenner potential can accurately predict the temperature dependence of specific heat, lattice constant, Grüneisen parameters and coefficient of thermal expansion (CTE) of diamond.     

Experimental investigation of high temperature thermal contact resistance with interface material

Thermal contact resistance plays a very important role in heat transfer efficiency and thermomechanical coupling response between two materials, and a common method to reduce the thermal contact resistance is to fill a soft interface material between these two materials. A testing system of high temperature thermal contact resistance based on INSTRON 8874 is established in the present paper, which can achieve 600°C at the interface. Based on this system, the thermal contact resistance between superalloy GH600 material and three-dimensional braid C/C composite material is experimentally investigated, under different interface pressures, interface roughnesses and temperatures, respectively. At the same time, the mechanism of reducing the thermal contact resistance with carbon fiber sheet as interface material is experimentally investigated. Results show that the present testing system is feasible in the experimental research of high temperature thermal contact resistance.     

Catalyst-free preparation of 1,2,4,5-tetrasubstituted imidazoles from a novel unexpected domino reaction of 2-azido acrylates and nitrones

A highly efficient and convenient method for the synthesis of 1,2,4,5-tetrasubstituted imidazoles from readily accessible 2-azido acrylates and nitrones has been developed. This reaction proceeded under mild conditions without the assistance of any metal, acid, or base.     

Theoretical studies on the transport property of oligosilane with p‐n junction

The electron transport properties of a novel p‐n junction nanowire caused by boron‐doping and phosphorus‐doping are investigated using density functional theory combined with the nonequilibrium Green's functions formalism. A satisfying rectification is observed. This is a reasonable result after the analysis of the molecular‐projected self‐consistent Hamitonian (MPSH) states, transmission spectra, the frontier orbitals, and the dipole moments. In contrast, the undoped chain has no rectification character. In addition, a negative differential resistance behavior is also observed at V = 1.8 ～ 2.2 V in the doped nanowire and it could be illustrated from the MPSH states and the transmission spectra. © 2011 Wiley Periodicals, Inc. Int J Quantum Chem, 2011