电喷印刷柔性传感器

柔性传感器因其在弯折、扭曲、拉伸等大变形条件下具有稳定的传感性能,所以在软体机器人、可穿戴电子和生物医疗等领域具有潜在的应用前景,受到了国内外研究者的广泛关注。与传统光刻技术相比,印刷技术制造作为增材制造,具有绿色、低成本和可大面积制造的优势,被广泛应用于柔性电子器件制备。其中,电流体动力喷墨打印(电喷印)技术因其具有多种功能材料的兼容性,被认为最有可能替代传统的光刻技术,实现柔性传感器高分辨率和跨规模制造。近年来,电喷印技术在微型化柔性传感器制造领域显示出广泛的应用潜力。本综述重点介绍了电喷印刷柔性传感器的工艺、材料和应用的最新研究进展。首先,详细介绍了电流体动力喷墨打印技术的工作原理,总结了用于电喷印的各种功能性墨水材料,然后,介绍了电喷印刷中墨水和柔性基底间表界面调控的问题。随后,综述了电喷印方法在柔性压力传感器、柔性气体传感器和柔性电化学传感器等柔性传感器制造的应用进展。最后,总结讨论了下一代电喷印刷技术在柔性传感器领域的机遇与挑战。     

基于铜金属有机配合物的热活化延迟荧光材料

具有热活化延迟荧光(thermally activated delayed fluorescence, TADF)特性的配合物可以同时利用单重态和三重态激子,因此发光量子效率较高,近年来受到广大科研工作者的关注。特别是铜金属有机配合物,最低单重态和最低三重态的能量差较小,又可以通过不同配体或取代基进行调节,所以具有较好TADF性能。本文根据配位原子的类型,汇总和分析了近5年具有TADF性质的铜配合物的结构特点和发光性能,并简要讨论了其在有机发光二极管(organic light-emitting diodes,OLEDs)中的潜在应用。     

In vivo Toxicity Evaluation of a Nano-drug Delivery System Using a Caenorhabditis elegansModel System

Drug carrier materials need to possess good biological safety. Presently, most biosafety evaluation studies use rodent animal models, including rats and rabbits. However, the cost of raising these animals is relatively high and the experimental period is long. Caenorhabditis elegans(C. elegans) presents an ideal toxicological evaluation model due to its simple structure, easy cultivation, short life cycle, and evolutionary conservation. In this paper, we used C. elegans to test the biological safety of our pH-responsive carrier system(FFPFF self-assembling into a nanosphere structure, FFPFF Nps), which was designed for anti-tumor drug delivery. Our results showed that exposure to high doses of FFPFF Nps did not have a significant impact on the survival rate, growth, development, movement, and reproduction of C. elegans. The preliminary evaluation of the overall biological model of C. elegans shows that FFPFF Nps has good biological safety and warrants further study.     

Stable Thiophene-sulfur Covalent Organic Frameworks for Oxygen Reduction Reaction(ORR)

Exploring novel materials deriving from earth resources to substitute for platinum(Pt) electrocatalyst to promote oxygen reduction reaction(ORR) of fuel cell cathode is very important. Herein, we have exploited two crystallographic thiophene-sulfur covalent organic frameworks(COFs), termed JUC-607 and JUC-608, as electrocatalysts that exhibited good ORR performances. These thiophene-sulfur COFs exhibited high stability, and their functional groups acting as active centers in the ORR can be precisely determined. Notably, due to a larger aperture for mass transfer and electrons transport, JUC-608 displayed a growing electrochemical performance, leading to a better ORR activity. Thus, this study will provide a new strategy for designing heteroatom-based COF materials for high-performance electrochemical catalysis.     

Accelerated kinetics of alkaline hydrogen evolution/oxidation reactions on dispersed ruthenium sites through N and S dual coordination

Efficient,robust and cost-effective electrocatalysts that catalyze hydrogen evolution/oxidation reaction(HER/HOR)in alkaline media are highly demanded.Recently,single-atom catalysts(SACs)have emerged as new promising candidates;however,the rational design of supports and the optimization of coordination environment between supports and metal atoms are challenging.In this work,we successfully fabricate atomically dispersed ruthenium(Ru)species,which are strongly coordinated by N and S dual heteroatoms on holey graphene(RuSA/NSG),as an excellent bifunctional catalyst for HER/HOR.In alkaline media,the developed catalyst exhibits high catalytic performance with a low overpotential of 57.3 mV to drive a current density of 10 mA cm^-1 for HER,and its mass activity is about 5.8 times higher than that of commercial Pt/C and Ru/C catalysts at an overpotential of 100 mV.Similarly,considerable HOR performance of Ru SA/NSG is verified to be superior to Pt/C and Ru/C.Furthermore,X-ray-based spectroscopy measurements and density-functional theory calculations have confirmed that,compared with Ru–N₄,the tailored Ru–N₄–S₂ with nearby S dopants can act as more active centers to greatly accelerate the sluggish HER/HOR kinetics in alkaline media.The present work provides a new atomic-level engineering strategy to modulate catalytic activities of SACs via the coordination design using dual heteroatoms on the carbon support.     

Simultaneous analysis of six inorganic anions in urine by double-suppress ion-exchange chromatography

This study is aimed to establish a simple, rapid, and accurate ion chromatography approach for the simultaneous detection of six inorganic anions in urine. Various performance parameters affecting the determination of anions were optimized, including the selection of sample protein precipitation agent, eluent, and flow rate. The final eluent was 3.6 mmol/L sodium carbonate and 12% isopropanol with a flow rate of 0.6 mL/min. Acetonitrile was used for pretreatment to precipitate proteins, and the volume ratio of urine to acetonitrile was 1:4. The correlation coefficient of the target anion calibration curve ranged from 0.9973 to 0.9999. The limit of detection ranged from 1.50 to 12.0 μg/L, and the method detection limit ranged from 15.0 to 120 μg/L. The standard recovery rate for low, medium, and high concentrations ranged from 90 to 110%. The inter-day and intra-day relative standard deviations were <5%. The method has high accuracy and good reproducibility and is suitable for the separation and determination of anions in urine.     

Theoretical Investigations on Photodissociation Dynamics of Deuterated Alkyl Halides CD3CH2F

The product branching ratio between different products in multichannel reactions is as important as the overall rate of reaction, both in terms of practical applications (\emph{e.g}. models of combustion or atmosphere chemistry) in understanding the fundamental mechanisms of such chemical reactions. A global ground state potential energy surface for the dissociation reaction of deuterated alkyl halide CD\begin{document}$ _3 $\end{document}CH\begin{document}$ _2 $\end{document}F was computed at the CCSD(T)/CBS//B3LYP/aug-cc-pVDZ level of theory for all species. The decomposition of CD\begin{document}$ _3 $\end{document}CH\begin{document}$ _2 $\end{document}F is controversial concerning C\begin{document}$ - $\end{document}F bond dissociation reaction and molecular (HF, DF, H\begin{document}$ _2 $\end{document}, D\begin{document}$ _2 $\end{document}, HD) elimination reaction. Rice-Ramsperger-Kassel-Marcus (RRKM) calculations were applied to compute the rate constants for individual reaction steps and the relative product branching ratios for the dissociation products were calculated using the steady-state approach. At the different energies studied, the RRKM method predicts that the main channel for DF or HF elimination from 1, 2-elimination of CD\begin{document}$ _3 $\end{document}CH\begin{document}$ _2 $\end{document}F is through a four-center transition state, whereas D\begin{document}$ _2 $\end{document} or H\begin{document}$ _2 $\end{document} elimination from 1, 1-elimination of CD\begin{document}$ _3 $\end{document}CH\begin{document}$ _2 $\end{document}F occurs through a direct three-center elimination. At 266, 248, and 193 nm photodissociation, the main product CD\begin{document}$ _2 $\end{document}CH\begin{document}$ _2 $\end{document}+DF branching ratios are computed to be 96.57%, 91.47%, and 48.52%, respectively; however, at 157 nm photodissociation, the product branching ratio is computed to be 16.11%. Based on these transition state structures and energies, the following photodissociation mechanisms are suggested: at 266, 248, 193 nm, CD\begin{document}$ _3 $\end{document}CH\begin{document}$ _2 $\end{document}F\begin{document}$ \rightarrow $\end{document}absorption of a photon\begin{document}$ \rightarrow $\end{document}TS5\begin{document}$ \rightarrow $\end{document}the formation of the major product CD\begin{document}$ _2 $\end{document}CH\begin{document}$ _2 $\end{document}+DF; at 157 nm, CD\begin{document}$ _3 $\end{document}CH\begin{document}$ _2 $\end{document}F\begin{document}$ \rightarrow $\end{document}absorption of a photon\begin{document}$ \rightarrow $\end{document}D/F interchange of TS1\begin{document}$ \rightarrow $\end{document}CDH\begin{document}$ _2 $\end{document}CDF\begin{document}$ \rightarrow $\end{document}H/F interchange of TS2\begin{document}$ \rightarrow $\end{document}CHD\begin{document}$ _2 $\end{document}CHDF\begin{document}$ \rightarrow $\end{document}the formation of the major product CHD\begin{document}$ _2 $\end{document}+CHDF.     

Basis Sets Dependency in Constructing Spectroscopy-Accuracy Ab Initio Global Electric Dipole Moment Functions

Recently, more attention have been paid on the construction of dipole moment functions (DMF) using theoretical methods. However, the computational methods to construct DMFs are not validated as much as those for potential energy surfaces do. In this letter, using Ar...He as an example, we tested how spectroscopyaccuracy DMFs can be constructed using ab initio methods. We especially focused on the basis set dependency in this scenario, i.e., the convergence of DMF with the sizes of basis sets, basis set superposition error, and mid-bond functions. We also tested the explicitly correlated method, which converges with smaller basis sets than the conventional methods do. This work can serve as a pictorial sample of all these computational technologies behaving in the context of constructing DMFs.     

基于“透过表面接枝”方式制备低分散性和高接枝密度聚合物刷的研究

"透过表面接枝"(grafting-through)是一种聚合物表面改性的新方法,可以显著改善传统grafting-from和grafting-to方法接枝工艺的缺陷,获得兼具高接枝密度和低分散性的聚合物刷产物.本文采用布朗动力学模拟方法,模拟研究了grafting-through方法接枝聚合物刷过程中的主控因素,从微观动力学角度阐明其特有的链增长趋同化效应是保持产物聚合物刷较低分散性的主因.引发效率在grafting-through中可显著提高,且产物聚合物刷的分子量呈现泊松分布.此外,反应中保持高的单体通量,可以同时实现产物聚合物较长的平均链长和较低的分散性,有利于制备性能优异的改性材料.该研究对深入理解grafting-through接枝过程的动力学主控因素,促进grafting-through技术的推广和工艺的改进具有一定的理论指导意义.     

Photocatalytic removal of tetracycline by a Z-scheme heterojunction of bismuth oxyiodide/exfoliated g-C3N4: performance,mechanism, and degradation pathway

Antibiotics, once being released into the environment, become recalcitrant organic pollutants, which pose a potential risk to ecological balance and human health. In this study, a Z-scheme heterojunction of bismuth oxyiodide (BiOI)/exfoliated g-C₃N₄ (BiOI/ECN hereafter) was synthesized by the combination of thermal exfoliation of g-C₃N₄ and chemical precipitation of BiOI for efficient photocatalytic degradation of tetracycline in aqueous solutions under visible light irradiation. The optimized BiOI/ECN delivered an outstanding degradation rate at circa 0.0705 min^?1, which was 10 times higher than that of the bulk g-C₃N₄. The photocatalytic degradation efficiency of tetracycline remained almost unchanged in a pH range of 3–11, and the BiOI/ECN displayed an excellent photostability upon recycled usage. The photocatalytic mechanism of tetracycline was ascribed to the main reactive oxidation species of photogenerated holes and superoxide radicals. In addition, the possible degradation pathways of tetracycline were investigated by HPLC-MS to identify intermediates. The toxicity of photocatalytic-generated intermediates of tetracycline was found significantly alleviated according to the calculation of quantitative structure–activity relationship prediction. This work not only provides an attractive photocatalyst for the removal of tetracycline but also opens a new avenue for rational design of Z-scheme heterojunction composites for tetracycline degradation.