Electrochemical behavior of uranyl in ionic liquid 1-butyl-3-methylimidazolium chloride mixture with water

Electrochemical behaviors of U(VI) in 1-butyl-3-methylimidazolium chloride (C₄MimCl) with various water contents investigated by chronopotentiometry and cyclic voltammetry. The electrochemical reduction of U(VI) was identified to follow two processes: a lower valence intermediate U(V) was initially formed at the potential of ca. ?0.2 V(vs. Ag wire). Then, further deposition of UO₂ was followed at around ?0.8 V. Little amount of water (1–4 wt%) in C₄MimCl, however, has an effect on the U(VI) reduction by changing the current density of the redox reaction and the diffusion coefficient of U(VI) in C₄MimCl. The deposited product by potentiostatic electrolysis on the surface of stainless steel electrode was characterized by the scanning electron microscopy (SEM), energy dispersive X-ray (EDX) and X-ray diffraction (XRD) methods. Although the electrodeposited black film was amorphous, the electrochemical reduced product of U(VI) can be still confirmed to be UO₂ by XRD after the crystallization of the amorphous deposits at 1,073 K in nitrogen atmosphere.     

The effect of cation size (H+, Li+, Na+, and K+) on McLafferty-type rearrangement of even-electron ions in mass spectrometry

Protonation and alkali-metal cation adduction are the most important ionization processes in soft-ionization mass spectrometry.Studies on the fragmentation mechanism of protonated and alkali-metal-cationized compounds in tandem mass spectrometry are essential and helpful for structural analysis.In some cases,it was often observed that a compound attached by different alkali-metal cations(or proton)exhibits similar fragmentation patterns but the relative abundances of product ions are different.This difference was considered to derive from the different electrostatic interactions of alkali-metal cations(or the bonded effect of proton)with the analyte.The alkali-metal cation with a smaller ionic radius shows stronger electrostatic interaction with the molecule because of its higher charge density.In addition,the bonded effect of the proton is stronger than the electrostatic interaction of the alkali-metal cation.In the present study,which used McLafferty-type rearrangements of even-electron ions([M+Cat]+,Cat=H,Li,Na,K)as model reactions,the effect of cation size in mass spectrometric fragmentation reactions is highlighted.These considerations were also successfully applied to interpret the similar but distinct fragmentation behavior of proton and alkali-metal cation adducts of a synthetic compound(2-(acetamido(phenyl)methyl)-3-oxobutanoate)and a drug(entecavir).     

A realization of digital wireless transmission for MRI signals based on 802.11b

In this paper, a digital wireless transmission system based on 802.11b standard for magnetic resonance imaging (MRI) application is designed and built for the first time to eliminate the interference aroused by coil array cables. The analysis shows that the wireless receiver has a very high sensitivity to detect MRI signals. The modulation technique of differential quadrature phase shift keyed (DQPSK) can be applied to MRI data transmission with rate of 2 Mbps and bandwidth of 2 MHz. The bench test verifies that this wireless link has a dynamic range over 86 dB supporting up to 3 T MRI system data transmission. The 2D spin echo imaging of phantom is performed and the SNR of the image obtained by the wireless transmission can be comparable with that got by the coaxial cables.     

A novel imaging tool for hepatic portal system using phase contrast technique with hydrogen peroxide‐generated O2 gas

The objective of this study was to investigate the potential of hydrogen peroxide‐generated oxygen gas‐based phase contrast imaging (PCI) for visualizing mouse hepatic portal veins. The O₂ gas was made from the reaction between H₂O₂ and catalase. The gas production was imaged by PCI in real time. The H₂O₂ was injected into the enteric cavity of the lower sigmoid colon to produce O₂ in the submucosal venous plexus. The generated O₂ gas could be finally drained into hepatic portal veins. Absorption contrast imaging (ACI) and PCI of O₂‐filled portal veins were performed and compared. PCI offers high resolution and real‐time visualization of the O₂ gas production. Compared with O₂‐based ACI, O₂‐based PCI significantly enhanced the revealing of the portal vein in vivo. It is concluded that O₂‐based PCI is a novel and promising imaging modality for future studies of portal venous disorders in mice models.     

基于阿秒抖动光纤锁模激光器的时钟同步

光纤锁模激光器结构简单, 运转稳定, 且输出的超短脉冲序列具有极高的时钟稳定性, 在抽运探测、脉冲相干合成等要求高精度时钟同步的前沿领域有着广阔的应用前景. 本文通过激光器腔内的电光调制器进行反馈控制, 实现了两台光纤锁模激光器之间的紧密时钟信号同步; 并且通过平衡光学互相关方法, 对残余的时钟误差信号进行了测量, 分辨率达到了13 as. 通过优化激光器的腔内动力学过程及反馈环路的参数, 在[1 Hz, 10 MHz]的积分区间内得到了109 as的残余时钟误差, 对应单台激光器的平均时间抖动为77 as.     

Synthesis and Characterizations of Strongly Phosphorescent Copper(I) Halide Complexes with Bridged Bis[2-(diphenylphosphino)phenyl]ether Ligand

A series of strongly phosphorescent copper(I) halide complexes, namely [Cu(μ-X)POP]₂ (X = Cl (1), Br (2), I (3), Br_0.5Cl_0.5 (4), POP = bis[2-(diphenylphosphino)phenyl]ether), have been synthesized by reacting CuX with the diphosphine ligand in 1:1 molar ratio. All complexes were characterized by spectroscopic analysis (IR, UV–Vis), elemental analysis, and photoluminescence study. Single-crystal X-ray diffraction revealed that complex 2 is a dinuclear structure which is constructed by two μ-X bridges and two POP ligands as μ₂ bridges. Other complexes were determined as isologues of complex 2 by powder X-ray diffraction and elemental analysis. All complexes exhibit intense blue-green phosphorescence with a lifetime of ~1 μs in the solid state. The halogen-mixed complex presents a lightly change in the luminescence comparing to that of parent complexes. The excited states of all complexes have been assigned as halide-to-ligand charge transfer state mixed metal-to-ligand charge transfer character based on the time-dependent density functional theory calculations. All complexes are thermally stable according to thermogravimetric analysis so that they are suitable for applying in luminescent devices.     

Synthesis and acaricidal activity of strobilurin-pyrimidine derivatives简

Pyriminostrobin, a new acaricide, was discovered in our previous studies. Because introducing fluorine into organic compounds can increase bioactivity, pyriminostrobin was modified as a series of strobilurin-pyrimidine derivatives for biological screening. The compounds were characterized by 1H NMR, MS and elemental analysis. Preliminary bioassays demonstrated that compounds 7e and 7i exhibited significant control against Tetranychus cinnabarinus （Boisd.） at 0.625 mg L^-1, and their acaricidal potencies were higher than pyriminostrobin in a greenhouse. The relationship between structure and acaricidal activity was also studied.     

Highly Selective CO2 Electroreduction to CH4 by In Situ Generated Cu2O Single-Type Sites on a Conductive MOF: Stabilizing Key Intermediates with Hydrogen Bonding

It is still a great challenge to achieve high selectivity of CH₄ in CO₂ electroreduction reactions (CO₂RR) because of the similar reduction potentials of possible products and the sluggish kinetics for CO₂ activation. Stabilizing key reaction intermediates by single type of active sites supported on porous conductive material is crucial to achieve high selectivity for single product such as CH₄. Here, Cu₂O(111) quantum dots with an average size of 3.5 nm are in situ synthesized on a porous conductive copper-based metal–organic framework (CuHHTP), exhibiting high selectivity of 73 % towards CH₄ with partial current density of 10.8 mA cm⁻² at −1.4 V vs. RHE (reversible hydrogen electrode) in CO₂RR. Operando infrared spectroscopy and DFT calculations reveal that the key intermediates (such as *CH₂O and *OCH₃) involved in the pathway of CH₄ formation are stabilized by the single active Cu₂O(111) and hydrogen bonding, thus generating CH₄ instead of CO.     

Hybrid Copolymerization via the Combination of Proton Transfer and Ring-opening Polymerization

Phosphazene base,t-BuP2,was employed to catalyze the proton transfer polymerization(PTP)of 2-hydroxyethyl acrylate(HEA),and PTP was further combined with ring-opening polymerization(ROP)to exploit a new type of hybrid copolymerization.The studies on homopolymerization showed that t-BuP2 was a particularly efficient catalyst for the polymerization of HEA at room temperature,giving an excellent monomer conversion.Throughout the polymerization,transesterification reactions were unavoidable,which increased the randomness in the structures of the resulting polymers.The studies on copolymerization showed that t-BuP2 could simultaneously catalyze the hybrid copolymerization via the combination of PTP and ROP at 25°C.During copolymerization,HEA not only provided hydroxyl groups to initiate the ROP ofε-caprolactone(CL)but also participated in the polymerization as a monomer for PTP.The copolymer composition was approximately equal to the feed ratio,demonstrating the possibility to adjust the polymeric structure by simply changing the monomer feed ratio.This copolymerization reaction provides a simple method for synthesizing degradable functional copolymers from commercially available materials.Hence,it is important not only in polymer chemistry but also in environmental and biomedical engineering.     

Unraveling the Impact of Gold(I)–Thiolate Motifs on the Aggregation‐Induced Emission of Gold Nanoclusters

Aggregation‐induced emission (AIE) provides an efficient strategy to synthesize highly luminescent metal nanoclusters (NCs), however, rational control of emission energy and intensity of metal NCs is still challenging. This communication reveals the impact of surface Au^I‐thiolate motifs on the AIE properties of Au NCs, by employing a series of water‐soluble glutathione (GSH)‐coordinated Au complexes and NCs as a model ([Au₁₀SR₁₀], [Au₁₅SR₁₃], [Au₁₈SR₁₄], and [Au₂₅SR₁₈]^?, SR=thiolate ligand). Spectroscopic investigations show that the emission wavelength of Au NCs is adjustable from visible to the near‐infrared II (NIR‐II) region by controlling the length of the Au^I‐SR motifs on the NC surface. Decreasing the length of Au^I‐SR motifs also changes the origin of cluster luminescence from AIE‐type phosphorescence to Au⁰‐core‐dictated fluorescence. This effect becomes more prominent when the degree of aggregation of Au NCs increases in solution.