The interaction of outgoing echolocation pulses and echoes in the false killer whale's auditory system: evoked-potential study

Brain auditory evoked potentials (AEP) associated with echolocation were recorded in a false killer whale Pseudorca crassidens trained to accept suction-cup EEG electrodes and to detect targets by echolocation. AEP collection was triggered by echolocation pulses transmitted by the animal. The target was a hollow aluminum cylinder of strength of -22 dB at a distance from 1 to 8 m. Each AEP record was obtained by averaging more than 1000 individual records. All the records contained two AEP sets: the first one of a constant latency and a second one with a delay proportional to the distance. The timing of these two AEP sets was interpreted as responses to the transmitted echolocation pulse and echo, respectively. The echo-related AEP, although slightly smaller, was comparable to the outgoing click-related AEP in amplitude, even though at a target distance as far as 8 m the echo intensity was as low as -64 dB relative to the transmitted pulse in front of the head. The amplitude of the echo-related AEP was almost independent of distance, even though variation of target distance from 1 to 8 m influenced the echo intensity by as much as 36 dB.     

On a final value problem for fractional reaction-diffusion equation with Riemann-Liouville fractional derivative

In this paper, we study a backward problem for a fractional diffusion equation with nonlinear source in a bounded domain. By applying the properties of Mittag-Leffler functions and Banach fixed point theorem, we establish some results above the existence, uniqueness, and regularity of the mild solutions of the proposed problem in some suitable space. Moreover, we also show the ill-posedness of our problem in the sense of Hadamard. The regularized solution is given, and the convergence rate between the regularized solution and the exact solution is also obtained.     

Highly efficient ammonia synthesis at low temperature over a Ru–Co catalyst with dual atomically dispersed active centers

The desire for a carbon-free society and the continuously increasing demand for clean energy make it valuable to exploit green ammonia (NH₃) synthesis that proceeds via the electrolysis driven Haber–Bosch (eHB) process. The key for successful operation is to develop advanced catalysts that can operate under mild conditions with efficacy. The main bottleneck of NH₃ synthesis under mild conditions is the known scaling relation in which the feasibility of N₂ dissociative adsorption of a catalyst is inversely related to that of the desorption of surface N-containing intermediate species, which leads to the dilemma that NH₃ synthesis could not be catalyzed effectively under mild conditions. The present work offers a new strategy via introducing atomically dispersed Ru onto a single Co atom coordinated with pyrrolic N, which forms RuCo dual single-atom active sites. In this system the d-band centers of Ru and Co were both regulated to decouple the scaling relation. Detailed experimental and theoretical investigations demonstrate that the d-bands of Ru and Co both become narrow, and there is a significant overlapping of t_2g and e_g orbitals as well as the formation of a nearly uniform Co 3d ligand field, making the electronic structure of the Co atom resemble that of a “free-atom”. The “free-Co-atom” acts as a bridge to facilitate electron transfer from pyrrolic N to surface Ru single atoms, which enables the Ru atom to donate electrons to the antibonding π* orbitals of N₂, thus resulting in promoted N₂ adsorption and activation. Meanwhile, H₂ adsorbs dissociatively on the Co center to form a hydride, which can transfer to the Ru site to cause the hydrogenation of the activated N₂ to generate N₂H_x (x = 1–4) intermediates. The narrow d-band centers of this RuCo catalyst facilitate desorption of surface *NH₃ intermediates even at 50 °C. The cooperativity of the RuCo system decouples the sites for the activation of N₂ from those for the desorption of *NH₃ and *N₂H_x intermediates, giving rise to a favorable pathway for efficient NH₃ synthesis under mild conditions.

The desire for a carbon-free society and the continuously increasing demand for clean energy make it valuable to exploit green ammonia (NH₃) synthesis that proceeds via the electrolysis driven Haber–Bosch (eHB) process.     

Carbon-nitrogen bond activation of amines by rhodium(III) porphyrin complexes

Carbon-nitrogen bond activation of amines by rhodium porphyrin chloride has been achieved to give rhodium porphyrin alkyl complexes. Rhodium porphyrin hydride and rhodium porphyrin dimer were proposed as the intermediates in cleaving the C-N bond.     

Synthesis and structure of an air-stable hypervalent organobismuth (III) perfluorooctanesulfonate and its use as high-efficiency catalyst for Mannich-type reactions in water

An air-stable hypervalent organobismuth (III) perfluorooctanesulfonate was synthesized and characterized by spectroscopic and X-ray crystallographic techniques, and found to exhibit high catalytic efficiency towards one-pot Mannich-type reaction of ketones with aromatic aldehydes and aromatic amines in water. This catalyst also shows good recyclability and reusability. This catalytic system would provide a simple, efficient and ‘green’ avenue towards the synthesis of β-amino ketones.     

Luminescent cyclometalated alkynylgold(III) complexes with 6-phenyl-2,2'-bipyridine derivatives: synthesis, characterization, electrochemistry, photophysics, and computational studies

A novel class of luminescent gold(III) complexes containing various tridentate cyclometalating ligands derived from 6-phenyl-2,2'-bipyridine and alkynyl ligands, [Au(RC^N^N)(C≡C-R')]PF(6), has been successfully synthesized and characterized. One of the complexes has also been determined by X-ray crystallography. Electrochemical studies show a ligand-centered reduction originated from the cyclometalating RC^N^N ligands as well as an alkynyl-centered oxidation. The electronic absorption and photoluminescence properties of the complexes have also been investigated. In acetonitrile at room temperature, the complexes show intense absorption at higher energy region with wavelength shorter than 320 nm, and a moderately intense broad absorption band at 374-406 nm, assigned as the metal-perturbed intraligand π-π* transition of the cyclometalating RC(∧)N(∧)N ligand, with some charge transfer character from the aryl ring to the bipyridine moiety. Most of the complexes have been observed to show vibronic-structured emission bands at 469-550 nm in butyronitile glass at 77 K, assigned to an intraligand excited state of the RC^N^N ligand, with some charge transfer character from the aryl to the bipyridyine moiety. Insights into the origin of the absorption and emission have also been provided by density functional theory (DFT) and time-dependent density functional theory (TDDFT) calculations.     

Isolating and Probing the Hot Spot Formed between Two Silver Nanocubes

Out of the frying pan : Hot spots can greatly increase the sensitivity of surface‐enhanced Raman scattering, but they remain poorly understood. A new strategy based on plasma etching (see picture) can be used to isolate and exclusively probe the SERS‐active molecules adsorbed in the hot‐spot region between two silver nanocubes.

     

Asymmetric synthesis of anti-1,2-amino alcohols via the Borono-Mannich reaction: a formal synthesis of (-)-swainsonine

Chiral alpha-hydroxy aldehydes generated in situ by the ADH reaction of vinyl sulfones undergo a borono-Mannich reaction with beta-styrenyl boronic acid and primary amines to give anti-1,2-amino alcohols in high enantiomeric purities (83-95% ee). This new method allows much more rapid access to these valuable chiral building blocks that has been used in a short formal synthesis (10 synthetic steps from 4-penten-1-ol) of (-)-swainsonine.     

基于自洽输运理论的介观体系动态电导的研究

基于介观体系电子动态输运的自洽理论,讨论了介观结构的动态电导.作为该理论的应用,采用一介观相干平行板电容器模型来进行研究. 结果表明:体系的动态电导与外场频率和体系费米能有关,为一复数且有有限虚部. 当外场频率较小时,动态电导随费米能的变化所呈现的特性和直流情形非常相似,但是随着外场频率的增加,两者差异就变得非常明显,体系动态电导随外场频率的变化呈现一些峰值结构. 在给定体系费米能时,动态电导随着外场频率的变化而产生振荡,并且出现了负的电导虚部,电导虚部的正负表明了体系的电容特性和电感特性. 关键词： 自洽输运理论 相干平行板电容器 电导 介观体系