Latest ArticlesAnalytical chemistry plays an important role in the qualitive and quantitative analysis for molecules in the various circumstances, especially for the high-resolution analysis. The dual-comb spectroscopy (DCS) technology with the characteristics of high resolution, high sensitivity and instantaneous sampling exhibited a great potential in high-resolution in-situ spectral methods and has been active in the fields of spatial ranging, air composition analysis, reaction monitoring and so on. In this review, we will summarize the principle of DCS according to the different wavelength coverage and overview the applications of DCS in analytical chemistry.
Chemical fixation of CO2 into C1 source, as a general approach, can effectively alleviate the emission of greenhouse gasses. Whereas, the challenge posed by the need for efficient catalysts with high catalytic active sites still exists. In this work, we reported a series of new hexavanadate clusters, [(C6H6ON)2(C2H8N2)2(CH3O)6V6IVO8] (V6–1), [(C6H6ON)2(C3H10N2)2(CH3O)6V6IVO8] (V6–2), [(C6H6ON)2(C6H14N2)2(CH3O)6V6IVO8] (V6–3) and [(C6H6ON)2(C4H11N2O)2(CH3O)4V6IVO8] (V6–4), assembled by 2-aminophenol and four different kinds of Lewis bases (LB), ethanediamine (en), 1,2-diaminopropane, 1,2-cyclohexanediamine and N-(2-hydroxyethyl)ethylenediamine (ben) together. Among them, the basic unit {V6} cluster featured Z-shaped configuration represents a brand-new example of hexanuclear vanadium clusters. Remarkably, the catalytic tests demonstrated that V6–1 as catalyst displays high catalytic activity in the cycloaddition for the CO2 fixation into cyclic carbonates by virtue of open V sites. As expected, for oxidative desulfurization of sulfides, V6–1 also exhibits satisfied catalytic effectiveness. Furthermore, the recycling test confirmed that catalyst V6–1 may be a bifunctional heterogeneous catalyst with great promise for both CO2 cycloaddition and oxidative desulfurization reactions.
Polysubstituted pyrroles are very important scaffolds in many bioactive natural products and synthetic pharmaceuticals. Here, a new gold-catalyzed cycloaddition of alkynes with azadienes to access tetrasubstituted pyrroles is demonstrated. The neighboring hydroxylmethyl group serves a very important directing group through an addition/cycloaddition/elimination cascade. Diverse polysubstituted pyrroles were synthesized in good yields under mild conditions in one step, and tricyclic pyrrole containing heterocycles were easily obtained through derivatization.
Formic acid decomposition (FAD) is considered a promising hydrogen production route to facilitate the ambient storage and on demand release of hydrogen energy. To optimize the catalysts for FAD, efforts have been paid to explore the underlying reason for the varied catalytic activity among catalysts with similar composition but differed structure. However, such endeavors are highly challenging due to the deeply intermingled effects of electronic structure, particle size, and facets, etc. Herein, to separately evaluate the respective effects of these factors, a series of catalysts with the same surface electronic structure and different particle size was prepared by cation dipole adjustment method. The performance and characterization results showed that the catalysts with different sizes and facets exhibited similar intrinsic activity with deviation of less than 5%. However, they showed 252% deviation of site stability, indicating that only the optimized electronic structure could enhance the intrinsic activity and a smaller particle size could extend the catalyst's life.
Fungal infections are hazardous to human health that has drawn wide attention. In this work, a specific and sensitive method combing the recognition of aptamer to (1, 3)-β-D-glucan and tyramide signal amplification technology was proposed for the in situ fluorescence imaging of fungi. Fungi could be distinctly observed by fluorescence microscope rapidly. This method provides morphology and diagnostic information for identifying fungi. The combination of aptamer and tyramide signal amplification technology is a promising tool for the detection of fungi, bacteria and even eukaryotic cell with the virtue of biomarkers.
Although converting the greenhouse gasses carbon dioxide (CO2) into solar fuels is regarded as a convenient means of solar energy storage, the intrinsic mechanism on how the high chemical inertness linear CO2 molecules is activated and converted on a semiconductor oxide is still elusive. Herein, by creating the oxygen vacancies on the typical hexagonal tungsten oxide (WO3), we realize the continuous photo-induced CO2 reduction to selectively produce CO under light irradiation, which was verified by isotope labeling experiment. Detailed oxygen vacancies evolution investigation indicates that light irradiation can simultaneously induce the in-situ formation of oxygen vacancies on hexagonal WO3, and the oxygen vacancies promote the adsorption and activation of CO2 molecules, leading to the CO2 reduction to CO on the hexagonal WO3 via an oxygen vacancies-involved process. Besides, the existence of water further promotes the formation of CO2 reduction intermediate, further promote the CO2 photoreduction. Our work provides insight on the mechanism for converting CO2 into CO under light irradiation.
The development of effective Ru catalyst for ammonia synthesis is of important practical value and scientific significance because of the wide application of ammonia as a fertilizer and its promising applications in the renewable energy. Generally, ZrO2 was regarded as an inferior support for Ru catalyst used in ammonia synthesis. Here we prepare ZrO2 with monoclinic phase and carbon species from ZrCl4 following the preparation route of UiO-66 as well as ammonia treatment. Owing to the presence of a larger amount of hydrogen adsorption as well as the easier desorption of hydrogen species, the ill effect of hydrogen species on the nitrogen adsorption-desorption and ammonia synthesis can be effectively alleviated. The resulting ZrO2-supported Ru catalyst showed 4 times higher ammonia synthesis activity than the conventional Ru/ZrO2 obtained from zirconium nitrate.
We present the synthesis, characterization and photoluminescence properties of uranium-containing selenotungstate, [(UO2)3(SeO3)3Na5(H2O)6(SeW6O21)(SeW9O33)3]21–, which was isolated by a one-pot reaction of uranium nitrate with sodium tungstate and sodium selenite in a pH 5.2 aqueous solution at 90 ℃. In this study, the effect of the introduction of lone-electron pair containing heteroatoms on the structure is demonstrated, a three-layered heterometallic {Se3U3Na5} cluster is encapsulated by two different anionic building block units: three trivacant Keggin {B-α-SeW9O33} and one Anderson {SeW6O21}. To our knowledge, the {Se3U3Na5} cluster has never been observed in the polyoxometalate chemistry. The solid-state photoluminescence properties and lifetime decay behaviours of the title compound (1) have been measured at room temperature, and the photoluminescence spectrum displays the characteristic emission bands of corresponding uranyl cations. In addition, the photoluminescence quantum yield of 1 is 72%, which is almost three times that of starting material UO2(NO3)2.6H2O (27%). By using this strategy, we envision that an increasing number of assemblies with 'open' clusters may be designed and obtained, in which the exposed oxygen atoms show strong affinity towards metal ions, providing new opportunities to generate bigger clusters or to tune existing properties.
Simulating the structures and behaviors of living organisms are of great significance to develop novel multi-functional intelligent devices. However, the development of biomimetic devices with complex deformable structures and synergistic properties is still on the way. Herein, we propose a simple and effective approach to create the multi-functional stimuli-responsive biomimetic devices with independently pre-programmable colorful visual patterns, complex geometries and morphable modes. The metal organic framework (MOF)-based composite film acts as a rigidity actuation substrate to support and mechanically guide the spatial configuration of the soft chiral nematic liquid crystal elastomer (CLCE) sheet. We can directly program the structural color of the CLCE sheet by adjusting the thickness distribution without tedious chemical modification. By using this coordination strategy, we fabricate an artificial flower, which exhibits a synergistic effect of both shape transformation and color change like paeonia 'Coral Sunset' at different flowering stages, and can even perform different flowering behaviors by bending, twisting and curling petals. The assembled bionic flower is innovatively demonstrated to respond to local stimuli of humidity, heat or ultraviolet irradiation. Therefore, the spatial assembly of CLCE combined with functional MOF materials has a wide range of potential application in multi-functional integrated artificial systems.
Manganese dioxide (MnO2), a commonly find oxidant in both natural environment and industrial application, plays a crucial role for various organic compound degradation. Tuning the MnO2 crystal structure is a cost-effective strategy to boost the oxidation reactions, where the challenge remains due to lacking in-depth investigation of the crystal properties. Herein, MnO2 with different crystalline structures (x-MnO2) including α-, β- and δ- was prepared through the hydrothermal synthesis for a typical organic pollutant removal. The structural and degradation analysis indicated that the oxidation capacity was originated from Mn3+ and oxygen vacancies (OVs). The intrinsic relationships between oxidation performance and other physiochemical properties such as morphology and electrochemistry were thoroughly discussed, and positive correlations between oxidation capacity and electrochemical properties were found which eventually led to excellent oxidation performance via modulating the above-mentioned properties. Moreover, the K+ content was determined to be the most crucial role in manipulating the structure properties. This work offers a crystal-level insight into the relationship between the crystal structure and oxidative property, promoting rational design of highly efficient oxidant.
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