Triphenylene: A versatile molecular receptor

Since the late seventies, the search for new molecular receptors has been constant in perfecting the affinity and selectivity of recognition in different media. At present, a renewed interest in (host:guest) chemistry focuses on the molecular detection of specific targets such as biological, pollutant, toxic or explosive species. This review of triphenylene-based receptors outlines their recent contribution to molecular recognition. Two main structural approaches were investigated to transform a simple triphenylene moiety into a host for neutral aromatic compounds or cations, by tailoring multivalent molecules provided with or without a flatten cavity. The properties of different receptors are presented along with the latest synthetic methods to prepare high-value triphenylenes and the perspectives in the field of sensing. In addition, the role of functionalized triphenylenes in extended (host:guest) systems is illustrated by the main examples of discotic liquid crystals and porous coordination polymers involving this polyaromatic compound.     

小直径棒材超声横波检测仿真分析

采用超声水浸聚焦斜入射方式进行小棒材表面、近表缺陷检测时,声波在水/棒和棒/缺陷界面会发生反射、折射、散射、衍射及波形转换等一系列物理变换。此时缺陷可检性对声波入射条件十分敏感,常出现由于检测条件设置不当而导致缺陷漏检、误检的情况。为解决这一问题,本文针对小棒材超声斜入射检测中的主要参数——入射角和水距,开展声场及缺陷声响应仿真,研究检测参数对不同部位缺陷检测能力的影响,并对仿真结果进行试验验证。通过研究得到了检测水距、入射角度对缺陷检测能力的影响,并得到最优检测条件。试验验证结果表明研究制定的检测方案可有效检测出表面、近表面裂纹缺陷。     

利用可见-近红外-中红外超快光谱揭示离子交换法制备的少层MoS2中缺陷介导的载流子动力学

本文结合可见-近红外-中红外瞬态吸收光谱技术对离子交换法制备的少层MoS₂中缺陷介导的载流子动力学进行了详细的解析. 在近红外瞬态吸收光谱中观察到的宽带漂白信号表明少层MoS₂纳米片带隙中分布着大量的缺陷态. 实验结果明确揭示了载流子被缺陷态的快速捕获以及进一步的复合过程，证明带隙中的缺陷态对MoS₂光生载流子动力学过程起着至关重要的作用. 在中红外瞬态吸收光谱中观察到的正信号到负信号的转变进一步证实了在导带下小于0.24 eV处存在被载流子占据的缺陷态. 这些在少层MoS₂纳米片中存在的缺陷态可以作为有效的载流子捕获中心来辅助光生载流子在皮秒时间尺度内完成非辐射复合过程.     

Investigation on thermal conductivity of graphene/Si heterostructure with different defect ratios and sizes

The thermal conductivity (TC) of graphene/Si heterostructures with different defect ratios and sizes was investigated using the molecular dynamics method. As the defect ratio of heterostructure increased, the TC decreased first sharply and then slowly under a high temperature stage. The TC of heterostructure also showed a significant size effect. This phenomenon was explained by phonon dispersion and flip competition. The phonon density of states for the graphene heterostructure with different defect ratios and sizes was obtained to understand the thermal transport mechanism. Analysis showed that with the increase in the defect ratio and when the flexural modes of the heterostructure became weak, the longitudinal and transverse modes gradually dominated the phonon transport. This phenomenon can be explained that the Si atom vibration was harder in the vertical plane than that of graphene. The vibration mode hindered the heat carrier of graphene and affected heat transport to the heterostructure.     

Characteristic material parameters of CIGS solar cell related with device performance

CIGS solar cells with power conversion efficiency (PCE) in the range of 1.82%–12.30% were obtained by using two-step process, and were further analyzed through various measurement techniques. Material parameters showed diverse values and some trends depending on the device performance. The lower performance device showed small integrated PL intensity, short minority life time, larger defect density and lower activation energy, whereas the higher performance device showed opposite values. We investigated relationship between material parameters and PCE of solar cells, and found that some physical parameters such as integrated PL intensity, minority life time, defect density, and difference between band gap and activation energy (E_g-E_a), which all reflect defect states in bulk and at pn interface, are strongly related with PCE and would be used as a good indicator to evaluate device performance quickly.     

Plasmon-Enhanced Electrochemiluminescence at the Single-Nanoparticle Level

Plasmon-enhanced electrochemiluminescence (ECL) at the single-nanoparticle (NP) level was investigated by ECL microscopy. The Au NPs were assembled into an ordered array, providing a high-throughput platform that can easily locate each NP in sequential characterizations. A strong dependence of ECL intensity on Au NP configurations was observed. We demonstrate for the first time that at the single-particle level, the ECL of Ru(bpy)₃²⁺-TPrA was majorly quenched by small Au NPs (<40 nm), while enhanced by large Au ones (>80 nm) due to the localized surface plasmon resonance (LSPR). Notably, the ECL intensity was further increased by the coupling effect of neighboring Au NPs. Finite Difference Time Domain (FDTD) simulations conformed well with the experimental results. This plasmon enhanced ECL microscopy for arrayed single NPs provides a reliable tool for screening electrocatalytic activity at a single particle.     

Electrophoresis-Assisted Multilayer Assembly of Nanoparticles for Sensitive Lateral Flow Immunoassay**

Lateral flow immunoassay (LFIA) is a rapid, simple, and inexpensive point-of-need method. A major limitation of LFIA is a high limit of detection (LOD), which impacts its diagnostic sensitivity. To overcome this limitation, we introduce a signal-enhancement procedure that is performed after completing LFIA and involves controllably moving biotin- and streptavidin-functionalized gold nanoparticles by electrophoresis. The nanoparticles link to immunocomplexes forming multilayer aggregates on the test strip, thus, enhancing the signal. Here, we demonstrate lowering the LOD of hepatitis B surface antigen from approximately 8 to 0.12 ng mL⁻¹, making it clinically acceptable. Testing 118 clinical samples for hepatitis B showed that signal enhancement increased the diagnostic sensitivity of LFIA from 73 % to 98 % while not affecting its 95 % specificity. Electrophoresis-driven enhancement of LFIA is universal (antigen-independent), takes two minutes, and can be performed by an untrained person.     

高比能锂离子电池层状富锂正极材料改性策略研究进展

层状富锂材料具有超过250 mAh∙g⁻¹的高可逆比容量,被认为是下一代高比能锂离子电池最具商业化前景的正极材料之一。然而,层状富锂材料在实际应用之前仍需解决诸多挑战,如高电压氧释放、层状到岩盐相的结构变化、过渡金属离子迁移等结构劣化,并由此带来了较低的初始库伦效率、电压/容量的衰减以及循环寿命的不足。针对以上问题,进行层状富锂材料改性无疑是一种行之有效的方法。本综述全面介绍了层状富锂材料的结构、组分以及电化学性能,在此基础上对材料改性策略进行了系统阐述,详细介绍了体相掺杂、表面包覆、缺陷设计、离子交换和微结构调控等一系列改性策略的现状以及发展趋势,最终提出了高容量和长循环层状富锂材料和高比能锂离子电池的设计思路。     

Minimizing Temperature Bias through Reliable Temperature Determination in Gas-Solid Photothermal Catalytic Reactions

Enormous advances in photothermal catalysis have been made over the years, whereas the temperature assessment still remains controversial in the majority of photothermal catalytic systems. Herein, we methodically uncovered the phenomenon of temperature determination bias arising from prominent temperature differences in gas-solid photothermal catalytic systems, which extensively existed yet has been overlooked in most relevant cases. To avoid the interference of temperature bias, we developed a universal protocol for reliable temperature evaluation of gas-solid photothermal catalytic reactions, with emphasis on eliminating the temperature gradient and temperature fluctuation of catalyst layer via optimizing the reaction system. This work presents a functional and credible practice for temperature detection, calling attention to addressing the effects of temperature differences, and reassessing the actual temperature-based performances in gas-solid photothermal catalysis.     

Singlet Oxygen Induced Site-Specific Etching Boosts Nitrogen-Carbon Sites for High-Efficiency Oxygen Reduction

Targeted construction of carbon defects near the N dopants is an intriguing but challenging way to boost the electrocatalytic activity of N-doped carbon toward oxygen reduction reaction (ORR). Here, we report a novel site-specific etching strategy that features targeted anchoring of singlet oxygen (¹O₂) on the N-adjacent atoms to directionally construct topological carbon defects neighboring the N dopants in N-doped carbon (¹O₂−N/C). This ¹O₂−N/C exhibits the highest ORR half-wave potential of 0.915 V_RHE among all the reported metal-free carbon catalysts. Pyridinic-N bonded with a carbon pentagon of the neighboring topological carbon defects is identified as the primary active configuration, rendering enhanced adsorption of O₂, optimized adsorption energy of the ORR intermediates, and a significantly decreased total energy barrier for ORR. This ¹O₂-induced site-specific etching strategy is also applicable to different precursors, showing a tremendous potential for targeted construction of high-efficiency active sites in carbon-based materials.