Latest ArticlesIn this work, we developed a novel photoelectrochemical (PEC) sensor based on n-p organic semiconductor heterojunction for sensitive detecting MCF-7 cancer cells. BTA-C4Ph and PM6 were designed as photoactive materials to form n-p heterojunction, which greatly enhanced the photoelectric conversion efficiency. Antibody-modified magnetic nanoparticles were utilized to capture and separate MCF-7 cells from samples. Detection of MCF-7 is ascribed to the loading of MCF-7 onto BTA-C4Ph-PM6 modified electrode that resulted in the decrease of photocurrent intensity. The PEC immunosensor displayed a linear concentration ranging from 50 cell/mL to 1 × 104 cell/mL with a limit of detection (LOD) of 41 cell/mL (S/N = 3) for MCF-7. Additionally, the senor also exhibited good stability, excellent selectivity and prominent reproducibility. Furthermore, the sensor was successfully applied to detect MCF-7 in whole blood. This work illustrates that n-p heterojunction of organic semiconductor may find wide applications for the preparation of different photoelectrochemical sensors.
Naphthyridine-fused bisimidazolium salts were designed and synthesized for the first time. The study of the Cu(Ⅱ) and Pd(Ⅱ) complexes demonstrated that the deprotonated dicarbene ligands are rigid chelating C, C-ligands with strong electron-donating ability in analogy with the classic phenanthroline N, N-ligands.
Aromatic carboxylic acids (ACAs) may be as transformed key metabolites via gut microbiome for playing better pharmacological effects. However, it's rare to achieve high-specificity, high-sensitivity, and high-throughput detection simultaneously, especially, for tracing trace ACAs in gut microbiome. In this work, firstly, a novel dual-template and double-shelled molecularly imprinted 96-well microplates (DDMIPs) was designed and amplified signal for p-hydroxybenzoic acid (PBA) and 3, 4, 5-trimethoxycinnamic acid (TMA). Additionally, the DDMIPs and a stable isotope labeling derivatization (SILD) method combined with the ultra-high performance liquid chromatography triple quadrupole tandem mass spectrometry (UHPLC-TQ MS) was firstly stepwise integrated, achieving high-effective, high-sensitive, and high-throughput study of gut microbiome metabolism. The whole strategy showed lower limits of detections (LODs) up to 1000 folds than the traditional method, and revealed a more real metabolism-time profile of PBA and TMA by 3-step signal amplification. The platform also laid the foundation for fast, simple, high-selective, high-effective, and high-throughput metabolism and pharmacological research.
The cellular response to the complex extracellular microenvironment is highly dynamic in time and type of extracellular matrix. Accurately reconstructing this process and analyzing the changes in receptor conformation on the cell membrane surface and intracellular or intercellular signaling has been a major challenge in analytical chemistry and biophysical methodology. In this paper, a time-coded multi-concentration microfluidic chemical waveform generator was developed for the dynamic signaling probing with single-cell array of high temporal resolution, high throughput, and multi-concentration combination stimulation. Based on innovative microchannel structure, sophisticated external control methods and multiplexing technology, the system not only allowed for temporally sequential permutations of the four concentrations of stimuli (time code), but also generated pulsed and continuous waveforms at different frequencies in a highly controllable manner. Furthermore, the single-cell trap array was set up to efficiently capture cells in suspension, dramatically increasing throughput and reducing experiment preparation time. The maximum frequency of the platform was 1 Hz, and one cell could be stimulated at multiple frequencies. To show the ability of the system to investigate rapid biochemical events in high throughput, pulse stimulation and continuous stimulation of different frequencies and different time codes, combined with four concentrations of histamine (HA), were generated for probing G protein-coupled receptor (GPCR) signaling in HeLa cells. Then, statistical analysis was performed for the mean peak height and mean peak area of the cellular response. We believe that the time-coded multi-concentration microfluidic chemical waveform generator will provide a novel strategy for analytical chemistry, biophysics, cell signaling, and individualized medicine applications.
Neuromuscular blocking agents (NMBAs) are extensively used during anesthesia to improve surgical conditions by relaxing skeletal muscle movements. Rapid neuromuscular recovery after surgery is desirable to facilitate the recovery of muscle function and prevent residual blockade. Decamethonium (C10) is a classic NMBA, which has been restricted over the past decades ascribed to lack of a suitable antidote in clinic. Herein we used carboxylatopillar[6]arene (CP6A) to reverse neuromuscular blocker effect of C10 through direct host-guest encapsulation. NMR and isothermal titration calorimetry served to confirm the complexation between CP6A and C10 with robust affinity [(1.07 ± 0.14) × 107 L/mol]. The CP6A was further used as a reversal agent of C10, which facilitated to decrease C10 concentration in mice blood and excrete via urinary clearance, resulting in rapid recovery from muscle relaxation. These favorable outcomes might lead us to suggest that this supramolecular strategy could allow patients to regain lucidity much faster than spontaneous recovery from anesthesia.
MeOTf-catalyzed formal [4 + 2] annulation of styrene oxides with alkynes to afford polysubstituted naphthalenes has been realized, which undergoes sequential electrophilic cyclization/ring expansion. A range of substrates were tolerated in the formation of naphthalene derivatives with high regioselectivity in satisfactory yields. The reaction could also be carried out on gram scale.
Mn-Si-MEL zeolite was developed as a bi-functional adsorption-catalytic oxidation material for volatile organic compounds (VOCs) elimination due to its good hydrophobicity & good organophileproperty brought by the substitution of Mn for Al in zeolite and the superior catalytic oxidation property endowed by the existence of Mn species. Various Mn-Si-MEL samples were obtained by introducing Mn to MEL crystallization system via different ways. It was found the incorporated Mn ways have a significant effect on the behavior of Mn being involved in the crystallization of MEL and finally influenced the distribution of Mn in zeolite as well the physicochemical properties of product zeolite. The seeding method (Mn-S2(Seed)) is favorable for the good incorporation and uniform distribution of Mn in zeolite while both recrystallization method (Mn-S2(RC)) and direct synthesis method (Mn-S2(DH)) are favorable for obtaining more reducible Mn species and surface adsorbed oxygen species. The Mn amount incorporated into zeolite follows Mn-S2(RC) (1.96 wt%) > Mn-S2(Seed) (1.07 wt%) ≈ Mn-S2(DH) (0.97 wt%), the adsorption capacity of various samples follows Mn-S2(Seed) (83.3 μmol/g) ≈ Mn-S2(RC) (82.1 μmol/g) > Mn-S2(DH) (76.1 μmol/g), while the catalytic oxidation ability of three samples follows Mn-S2(RC) ≈ Mn-S2(DH) > Mn-S2(Seed). Furthermore, Mn-S2(RC) which exhibits both superior adsorption capacity and catalytic oxidation ability shows good hydrophobicity and superior recyclability, demonstrating its great potential to be applied in the VOCs elimination by an enrichment-degradation route.
The catalytic elimination of nitrogen-containing volatile organic compounds (NVOCs) still encounters bottlenecks in NOx formation and low N2 selectivity. Here, a series of Cu-promoted Ce-Zr mixed oxide catalysts were synthesized using a simple precipitation approach, and n-butylamine was adopted as the probe pollutant to evaluate their catalytic performance. The CeCu10%ZrOx catalyst exhibited the best catalytic activity, with 100% n-butylamine conversion and 90% N2 selectivity at 250 ℃. Concurrently, this sample also displayed good water resistance. A detailed characterization of the catalyst was performed through a series of experimental studies and theoretical calculations. The addition of Cu increased the redox property and promoted the production of oxygen vacancies, all of which were favorable for the greatest n-butylamine selective catalytic oxidation performance. The changes of oxygen vacancies over CeCu10%ZrOx in reaction process were studied by in situ Raman spectra. Moreover, in situ diffuse reflectance infrared Fourier transform spectra (DRIFTs) and theoretical calculations were employed to explore the reaction mechanism of n-butylamine selective oxidation. The high activity and selectivity of this catalyst confirm the practical feasibility of the selective oxidation of n-butylamine to CO2 and N2, and the exploration of the reaction mechanism provides new insights into the further design of catalysts.
Sophoralines A-C, three novel [2 + 2] cycloaddition dimers of matrine-based alkaloids with an unprecedented 6/6/6/6/4/6/6/6/6 nonacyclic skeleton containing 11 stereogenic centers, were isolated from Sophora alopecuroides. Their structures were determined by spectroscopic methods, and the absolute configurations were further determined by single-crystal X-ray diffraction analysis for 1 and quantum chemical calculations of electronic circular dichroism (ECD) spectra for 2 and 3. Moreover, 1 exhibited excellent hepatoprotective activities in acetaminophen-induced liver injury in vitro and in vivo.
Selective hydrogenation of substituted nitroarenes is an important reaction to obtain amines. Supported metal catalysts are wildly used in this reaction because the surface structure of supports can tune the properties of the supported metal nanoparticles (NPs) and promote the selectivity to amines. Herein, Pt NPs were immobilized on FeOOH, Fe3O4 and α-Fe2O3 nanorods to synthesize a series of iron compounds supported Pt catalysts by liquid phase reduction method. Chemoselective hydrogenation of 3-nitrostyrene to 3-aminostyrene was used as probe reaction to evaluate the performance of the catalysts. The results show that Pt/FeOOH exhibits the highest selectivity and activity. FeOOH support with pores and -OH groups can tune the electronic structure of Pt NPs. The positive charge of Pt NPs supported on FeOOH is key factor for improving the catalytic performance.
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