摘要：A series of naphthalimide azoles as potential antibacterial and antifungal agents were conveniently and efficiently synthesized starting from commercially available 6-bromobenzo[de]isochromene-l,3-dione. All the new compounds were characterized by NMR, IR, MS and HRMS spectra. Their antimicrobial activities were evaluated against four Gram-positive bacteria, four Gram-negative bacteria and two fungi using two-fold serial dilution technique. The biological assay indicated that most of the prepared compounds exhibited inhibition to the tested strains. In particular, the triazolium derivatives not only gave higher ef- ficacy than their corresponding precursory azoles, but also demonstrated comparable or even better potency than the reference drugs Chloromycin, Orbifloxacin and Fluconazole. Some factors including structural fragments, pH and ClogP values of the target molecules were also preliminarily discussed.

摘要：Atomically precise gold cluster catalysts have emerged as a new frontier in catalysis science,owing to their unexpected catalytic *** this work,we explore the evolution of the catalytic activity of clusters formed by the structural fusion of icosahedral Au13 units,namely Au25(SR)18,Au38(SR)24,and Au25(PPh3)10(SC2H4Ph)5Cl2,in the oxidation of pyrrolidine toγ-*** demonstrate that the structural fusion of icosahedral Au13 units,forming vertex-fused(vf),face-fused(ff),and body-fused(bf)clusters,can induce a decrease in the catalytic activity in the following order:Aubf>Auff>*** structural fusion of icosahedral Au13 units in the clusters does not distinguish the adsorption modes of pyrrolidine over the three clusters from each other,but modulates the chemical adsorption capacity and electronic properties of the three clusters,which is likely to be the key reason for the observed changes in catalytic *** results are expected to be extendable to study and design atomically defined catalysts with elaborate structural patterns,in order to produce desired products.

摘要：An expedient and economic approach for constructing O,O,N-spiro compounds consisting of both a 1,3-oxazine and a furan ring through a catalyst-free formal[4+1]/[4+2]cycloaddition cascade sequence of isocyanides with two molecules of acylketene formed in situ through thermal-induced Wolff rearrangement of 2-diazo-1,3-diketones was *** reaction displayed good functional group tolerance and was compatible with different isocyanides and 2-diazo-1,***,preliminary asymmetric attempts of this reaction are made by utilizing optically pure isocyanides as inputs,and moderate diastereomeric induction was observed.

摘要：Recently, the power conversion efficiencies(PCEs) of all-polymer solar cells(all-PSCs) have increased rapidly. To further increase the PCE of all-PSCs, it is necessary to create new donor polymers matching the polymer acceptors. In this paper, we synthesize a new quinoxaline-based polymer donor PBQ8 with n-octyl side chain on the quinoxaline unit, which possesses the same skeleton structure to the previously reported PBQ5(with isooctyl side chain). The effects of alkyl side chains on the physicochemical properties of the polymer donor were investigated. In comparison with PBQ5, PBQ8 exhibits stronger intermolecular interactions and better molecular packing. When blending with polymer acceptor PY-IT, the PBQ8:PY-IT based devices demonstrated a higher PCE value of 17.04%, which is one of the highest PCEs occurred in the all-PSCs. And the PBQ5:PY-IT(PCE 15.56%, Voc0.907 V, FF 69.72%, and Jsc24.60 m A cm^(-2)) is much lower. The PBQ8:PY-IT blend displayed more efficient exciton dissociation, better molecular stacking properties, preferable phase separation and higher mobility. These indicate that as an effective method, side chain engineering can improve the efficiency of the all-PSCs.

摘要：Modification of classic fluorophore to possess the emission transitions between aggregation-induced emission （ALE） and intrinsic emission offers reliable approach to the design of ratiometric fluorescent sensors. In this study, a proton acceptor benzimidazole was integrated with BODIPY to form three compounds, BBI-1/2/3, which demonstrated the AIE （-595 nm, Iagg） in neutral aqueous medium and intrinsic BODIPY emission （-510 nm,Iint） in acidic medium. All the three showed the ratiometric pH sensing behavior in a dual excitation/dual emission mode, yet BBI-3 displayed still the dual emission ratiometric pH sensing ability. The pH-dependent emission ratio/int/Iagg of the three were fully reversible, and no interference was observed from normal abundant chemical species in live cells. Their different pKa （BBI-1, pKa 4.4; BBI-2, pKa 2.7; BBI-3, pKa 3.6） suggested that the substituents on benzimidazole moiety were essential to govern their functioning pH range. The ratiometric imaging of BBI-1 in A549 cells provided an effective intracellular pH （pHi） calibration formula corresponding to emission ratio oflJ Iint/Iagg. Ratiometric pH imaging in A549 cells upon small particle exposure confirmed the particle-induced cellular acidification with this formula. Both particle size and the chemical nature of the particle contribute to the observed acidification effect. The synchronization of lysosome disruption to cellular acidification in A549 cells upon crystalline silica exposure was directly observed for the first time with BBI-1, showing the potential application of BBI-1 in the study of silicosis and other related diseases. This study de- monstrated that endowing fluorophore with AIE/intrinsic emission transition could be a promising strategy for ratiometric sensor design.

摘要：TiO_(2)is a promising photocatalyst with limited use in practical applications owing to its wide bandgap,narrow light response range,and rapid recombination of photoexcited *** address these limitations,a novel 1D/2D TiO_(2)/ZnIn_(2)S_(4)heterostructure was designed according to the principles of the S-scheme *** TiO_(2)/ZnIn_(2)S_(4)(TZISx)hybrids prepared via a hydrothermal method afforded significant improvement in photocatalytic hydrogen evolution(PHE)in comparison to pristine TiO_(2)and ZnIn_(2)S_(4).In particular,the optimal TZIS2 sample(mass ratio of ZnIn_(2)S_(4)to TiO_(2)was 0.4)exhibited the highest PHE activity(6.03 mmol/h/g),which was approximately 3.7 and 2.0 times higher than those of pristine TiO_(2)and ZnIn_(2)S_(4),*** improvement in the PHE of the TZIS2 sample could be attributed to the formation of an intimate heterojunction interface,high-efficiency separation of charge carriers,abundant reactive sites,and enhanced light absorption ***,theoretical and experimental results demonstrated that the S-scheme mechanism of interfacial electron transfer in the TZISx composites facilitated the transfer and separation of photoexcited charge carriers,resulting in more isolated photoexcited electrons for the PHE reaction.

摘要：The initial efficiency is a very important criterion for carbon anode material of Li-ion *** relationship between initial efficiency and structure parameters of carbon anode material of Li-ion battery was investigated by an artificial intelligence approach called Random Forests using D10,D50,D90,BET specific surface area and TP density as inputs,initial efficiency as *** results give good classification performance with 91%*** variable importance analysis results show the impact of 5 variables on the initial efficiency descends in the order of D90,TP density,BET specific surface area,D50 and D10;smaller D90 and larger TP density have positive impact on initial *** contribution of BET specific surface area on classification is only 18.74%,which indicates the shortcoming of BET specific surface area as a widely used parameter for initial efficiency evaluation.

摘要：A nanocomposite catalyst with a nonstoichiometric titanium oxide loaded on a special nanotubular alumina(γ‐Al2O3‐nt)was developed and used to reduce cinnamaldehyde to cinnamyl alcohol with sacrificial isopropanol,i.e.,a Meerwein‐Ponndorf‐Verley type *** deposition process produced a highly disperse layer of titanium oxide on the surface of aγ‐Al2O3‐nt *** a reduction treatment,the as‐prepared TiOx/γ‐Al2O3‐nt was a highly efficient catalyst for the hydrogen transfer reaction between isopropanol and *** for cinnamic alcohol was higher than99%and the conversion of cinnamaldehyde was higher than95%.The regular morphology of theγ‐Al2O3‐nt support with homogeneous surface sites and the uniformly dispersed titanium oxide featured a high concentration surface Ti(III)*** factors contributed to the high performance of the TiOx/γ‐Al2O3‐nt catalyst.

摘要：Heterostructure engineering holds exceptional promise for the development of high-performance electrocatalysts for overall water ***,production of inexpensive and high-efficiency bifunctional electrocatalysts remains a ***,we demonstrate a simple method to synthesize a paper-mulberry(Broussonetia papyrifera)-inspired Co_(9)S_(8)@CoNi_(2)S_(4)/nickel foam(Co_(9)S_(8)@CoNi_(2)S_(4)/NF)heterojunction with high catalytic activity and *** process involves in situ growth of NiCo layered double hydroxide and in situ derivatization of ZIF-67,followed by the S heteroatom *** Co_(9)S_(8)@CoNi_(2)S_(4)/NF benefits from the heterostructure and functional advantages of multidimensional building blocks including one-dimensional(1D)nanowires,2D nanosheets and *** optimized Co_(9)S_(8)@CoNi_(2)S_(4)/NF heterojunction with 10% sulphur content reveals excellent electrocatalytic activity with the lower overpotentials of 68 mV for hydrogen evolution reaction(HER)and 170 mV for oxygen evolution reaction(OER)at 10 mA cm^(-2) in the 1.0 mol L^(-1) KOH solution,which is superior to the recently reported transition metal based *** outstanding performance is attributed to the strong interface coupling between CoNi_(2)S_(4) and Co_(9)S_(8),the advantage of multidimensional structure and the customized electronic *** density functional theory suggests that the interface between Co_(9)S_(8) and CoNi_(2)S_(4) optimizes the adsorption of the multiple intermediates and further facilitates water splitting *** work offers a generic approach for heterostructure engineering design of highperformance catalytic system applications.

摘要：Unveiling the active site of an electrocatalyst is fundamental for the development of efficient electrode *** the two-electron water oxidation to produce H_(2)O_(2),competitive reactions,including four-and one-electron water oxidation and surface reconstruction derived from the high-oxidative environment co-existed,leading to great challenges to identify the real active sites on the *** this work,Ti/TiO_(2)-based electrodes calcined under air,nitrogen,or urea atmospheres were selected as electrocatalysts for two-electron water *** analyses were applied to evaluate the catalytic activity and *** morphological and current change on the electrode surface were determined by scanning electrochemical microscopy,while the chemical and valence evolutions with depth distributions were tested by XPS combined with cluster argon ion *** results demonstrated that Ti/TiO_(2) nanotube arrays served as the support,while the functional groups of carbonyl groups and pyrrolic nitrogen derived from the co-pyrolysis with urea were the active sites for the H_(2)O_(2) *** finding provided a new horizon to design efficient catalysts for H_(2)O_(2) production.