Aggregation-induced Emission Materials for High-efficiency Perovskite Solar Cells

The perovskite solar cells (PSCs) with high efficiency and stability are in great demand for commercial applications. Although the remarkable photovoltaic feature of perovskite layer plays a great role in improving the PCE of PSCs, the inevitable defects and poor stability of perovskite, etc. are the bottleneck and restrict the commercialization of PSCs. Herein, a review provides a strategy of applying aggregation-induced emission (AIE) molecules, containing passivation functional groups and distinct AIE character, which serves as the alternative materials for fabricating high-efficiency and high-stability PSCs. The methods of introducing AIE molecules to PSCs are also summarized, including additive engineering, interfacial engineering, hole transport materials and so on. In addition, the functions of AIE molecule are discussed, such as defects passivation, morphology modulation, well-matched energy level, enhanced stability, hole transport ability, carrier recombination suppression. Finally, the detailed functions of AIE molecules are offered and further research trend for high performance PSCs based on AIE materials is proposed.     

Thermally Responsive Selenide-containing Materials Based on Transalkylation of Selenonium Salts

Covalent adaptable networks (CANs) possess unique properties as a result of their internal dynamic bonds, such as self-healing and reprocessing abilities. In this study, we report a thermally responsive C−Se dynamic covalent chemistry (DCC) that relies on the transalkylation exchange between selenonium salts and selenides, which undergo a fast transalkylation reaction in the absence of any catalyst. Additionally, we demonstrate the presence of a dissociative mechanism in the absence of selenide groups. After incorporation of this DCC into selenide-containing polymer materials, it was observed that the cross-linked networks display varying dynamic exchange rates when using different alkylation reagents, suggesting that the reprocessing capacity of selenide-containing materials can be regulated. Also, by incorporating selenonium salts into polymer materials, we observed that the materials exhibited good healing ability at elevated temperatures as well as excellent solvent resistance at ambient temperature. This novel dynamic covalent chemistry thus provides a straightforward method for the healing and reprocessing of selenide-containing materials.     

Catalytic transfer hydrogenation of biomass-derived furfural to furfuryl alcohol with formic acid as hydrogen donor over CuCs-MCM catalyst

Catalytic transfer hydroge nation(CTH) of furfural(FF) to furfu ryl alcohol(FFA) has received great intere st in recent years.He rein,Cu-Cs bimetallic supported catalyst,CuCs(2)-MCM,was developed for the CTH of FF to FFA using formic as hydrogen donor.CuCs(2)-MCM achieved a 99.6% FFA yield at an optimized reaction conditions of 170℃,1 h.Cu species in CuCs(2)-MCM had dual functions in catalytically decomposing formic acid to generate hydrogen and hydrogenating FF to FFA.The doping of Cs made the size of Cu particles smaller and improved the dispersion of the Cu active sites.Impo rtantly,the Cs species played a favorable role in enhancing the hydrogenation activity as a promoter by adjusting the surface acidity of Cu species to an appropriate level.Correlation analysis showed that surface acidity is the primary factor to affect the catalytic activity of CuCs(2)-MCM.     

Single Chlamydomonas reinhardtii cell separation from bacterial cells and auto-fluorescence tracking with a nanosieve device

A planar, transparent, and adaptable nanosieve device is developed for efficient microalgae/bacteria separation. In the proposed method, a sacrificial layer is applied with dual photolithography patterning to achieve a 1D channel with a very low aspect ratio (1:10 000). A microalgae/bacteria mixture is then introduced into the deformable PDMS nanochannel. The hydrodynamic deformation of the nanochannel is regulated to allow the bacteria cells to pass through while leaving the microalgae cells trapped in the device. At a flow rate of 4 μL/min, the supernatant collected from the device is indistinguishable from a control solution, indicating that nearly all the microalgae cells are trapped in the device. Additionally, this device is capable of single cell auto-fluorescence tracking. These microalgae cells demonstrate minimal photobleaching over 250 s laser exposure and could be used to monitor hazardous compounds in the sample with a continuous flow. This method will be valuable to purify microalgae samples containing contaminations and study single-cell heterogeneity.     

Inhibition of Thiol-Mediated Uptake with Irreversible Covalent Inhibitors

Thiol-mediated uptake is emerging as method of choice to penetrate cells. This study focuses on irreversible covalent inhibitors of thiol-mediated uptake. High-content high-throughput screening of the so far largest collection of hypervalent iodine reagents affords inhibitors that are more than 250 times more active than Ellman’s reagent and rival the best dynamic covalent inhibitors. Comparison with other irreversible reagents reveals that inhibition within one series follows reactivity, whereas inhibition across series deviates from reactivity. These trends support that molecular recognition, besides dynamic covalent exchange, contributes significantly to thiol-mediated uptake. The most powerful inhibitors besides the best hypervalent iodine reagents were Fukuyama’s nosyl protecting group and super-cinnamaldehydes that have been introduced as irreversible activators of the pain receptor TRPA1. Considering that several viruses use different forms of thiol-mediated uptake to enter cells, the identification of new irreversible inhibitors of thiol-mediated uptake is of general interest for the discovery of new antivirals.     

A Bifunctional B,N-Based Asymmetric Catalytic Nitrostyrene-Michael Addition Acting through a 10-Membered Ring Cyclic Transition State

The B,N-bifunctional catalyst homoboroproline has been applied to a catalytic asymmetric nitroalkene-Michael addition to β-nitrostyrene analogues, showing broad substrate tolerance, high conversions and moderate to good asymmetric induction. The ability of homoboroproline to act as an efficient catalyst based on enamine-formation of the secondary amine, coupled with intramolecular Lewis-acid chelation of the nitro function, in a non-FLP manner, to effect efficient and enantioselective catalysis via a proposed large 10-membered ring transition state is remarkable and reinforced by theoretical calculations.     

吲哚多样化环化合成咔唑衍生物研究进展

咔唑是一类特殊的含氮芳杂环分子,咔唑衍生物理化性质独特、结构多样,在天然产物、药物和功能材料领域有着广阔的应用,其合成方法一直备受关注.从吲哚直接环化到咔唑的合成方法简洁高效,原料廉价易得、产物种类多样.总结了近5年来以2,3-未取代吲哚为原料合成咔唑衍生物的方法,典型环化策略包含以下三种:[2+2′+2′]环化反应、[2+2′+2″]环化反应和[4+2]苯环化反应,探讨了每种方法的特点,并对未来的发展前景进行展望.     

多金属氧酸盐材料在二氧化碳电催化还原领域中的研究进展

随着工业发展和全球人口的持续增长,人类对化石燃料的消耗日益增加,从而导致大气中二氧化碳含量的显著增加以及与之相伴的一系列环境问题.电化学还原二氧化碳制备高附加值的燃料和化学品具有稳定的效率和较高的经济可行性等特点,目前已成为一种有前景的策略来缓解当前全球面临的能源短缺和气候变暖问题.然而,电催化二氧化碳还原过程存在反应能垒高和复杂的多电子/质子耦合过程等不足,因此,合理有效的电催化剂设计成为该领域的关键问题.近年,理解和明确电化学二氧化碳还原反应过程的活性起源、选择性调控机制和催化反应机理已成为高效电催化剂设计过程中的重要指导原则.作为一类独特的纳米尺度的金属氧簇,多金属氧酸盐(多酸)已成为二氧化碳还原领域的热点材料.尤其是,多酸明确的结构、优越的电子/质子存储转移能力和二氧化碳吸附活化能力有助于探究二氧化碳还原反应过程中的活性起源和构效机制.因此,利用多酸阐明电化学二氧化碳还原反应中的这些关键问题对于开发高效、可实用化的电催化剂意义重大.本文综述了近年多酸在电催化二氧化碳还原反应中取得的进展,重点介绍了多酸阴离子均相分子催化剂、多酸基无机-有机杂化材料催化剂、多酸电解质溶液、多酸-纳米复合材料在电催化二氧化碳还原反应中的应用.利用密度泛函理论结合原位实验证据推测了可能的反应机理,探讨了多酸对电催化活性和产物选择性的影响,揭示了电子/质子存储-转移过程和多酸表面修饰工程在电催化二氧化碳还原过程中的重要作用.最后,本文还分析了多酸基材料存在的问题与面临的挑战,并对多酸基材料在二氧化碳还原领域的未来发展进行了展望,这对理解电催化二氧化碳还原反应中的关键步骤和开发新型高效的电催化二氧化碳还原电催化剂具有启发意义.     

Contradictory effect of gold nanoparticle-decorated molybdenum sulfide nanocomposites on amyloid-β-40 aggregation

The effect of gold nanoparticle-decorated molybdenum sulfide (AuNP-MoS₂) nanocomposites on amyloid-β-40 (Aβ₄₀) aggregation was investigated. The interesting discovery was that the effect of AuNP-MoS₂ nanocomposites on Aβ₄₀ aggregation was contradictory. Low concentration of AuNP-MoS₂ nanocomposites could enhance the nucleus formation of Aβ₄₀ peptides and accelerate Aβ₄₀ fibrils aggregation. However, although high concentration of AuNP-MoS₂ nanocomposites could enhance the nucleus formation of Aβ₄₀ peptides, it eventually inhibited Aβ₄₀ aggregation process. It might be attributed to the interaction between AuNP-MoS₂ nanocomposites and Aβ₄₀ peptides. For low concentration of AuNP-MoS₂ nanocomposites, it was acted as nuclei, resulting in the acceleration of the nucleation process. However, the structural flexibility of Aβ₄₀ peptides was limited as the concentration of AuNP-MoS₂ nanocomposites was increased, resulting in the inhibition of Aβ₄₀ aggregation. These findings suggested that AuNP-MoS₂ nanocomposites might have a great potential to design new multifunctional material for future treatment of amyloid-related diseases.     

Inhibitor Development against p7 Channel in Hepatitis C Virus

Hepatitis C Virus (HCV) is the key cause of chronic and severe liver diseases. The recent direct-acting antiviral agents have shown the clinical success on HCV-related diseases, but the rapid HCV mutations of the virus highlight the sustaining necessity to develop new drugs. p7, the viroporin protein from HCV, has been sought after as a potential anti-HCV drug target. Several classes of compounds, such as amantadine and rimantadine have been testified for p7 inhibition. However, the efficacies of these compounds are not high. Here, we screened some novel p7 inhibitors with amantadine scaffold for the inhibitor development. The dissociation constant (Kd) of 42 ARD-series compounds were determined by nuclear magnetic resonance (NMR) titrations. The efficacies of the two best inhibitors, ARD87 and ARD112, were further confirmed using viral production assay. The binding mode analysis and binding stability for the strongest inhibitor were deciphered by molecular dynamics (MD) simulation. These ARD-series compounds together with 49 previously published compounds were further analyzed by molecular docking. Key pharmacophores were identified among the structure-similar compounds. Our studies suggest that different functional groups are highly correlated with the efficacy for inhibiting p7 of HCV, in which hydrophobic interactions are the dominant forces for the inhibition potency. Our findings provide guiding principles for designing higher affinity inhibitors of p7 as potential anti-HCV drug candidates.