Enhancing carrier transfer properties of Na-rich anti-perovskites, Na4OM2 with tetrahedral anion groups: an evaluation through first-principles computational analysis.

The practical application of Na-based solid-state electrolytes (SSEs) is limited by their low level of conduction. To evaluate the impact of tetrahedral anion groups on carrier migration, we designed a set of anti-perovskite SSEs theoretically based on the previously reported Na4OBr2, including Na4O(BH4)2, Na4O(BF4)2, and Na4O(AlH4)2. It is essential to note that the excessive radius of anionic groups inevitably leads to lattice distortion, resulting in asymmetric migration paths and a limited improvement in carrier migration rate. Na4O(AlH4)2 provides a clear example of where Na+ migrates in two distinct environments. In addition, due to different spatial charge distributions, the interaction strength between anionic groups and Na+ is different. Strong interactions can cause carriers to appear on a swing, leading to a decrease in conductivity. The low conductivity of Na4O(BF4)2 is a typical example. This study demonstrates that Na4O(BH4)2 exhibits remarkable mechanical and dynamic stability and shows ionic conductivity of 1.09 × 10-4 S cm-1, two orders of magnitude higher than that of Na4OBr2. This is attributed to the expansion of the carrier migration channels by the anion groups, the moderate interaction between carriers and anionic groups, and the "paddle-wheel" effect generated by the anion groups, indicating that the "paddle-wheel" effect is still effective in low-dimensional anti-perovskite structures, in which atoms are arranged asymmetrically.

A 3,5-dinitropyridin-2yl Substituted Flavonol-based Fluorescent Probe for Rapid Detection of H2S in Water, Foodstuff Samples and Living Cells.

A novel flavonol-based fluorescent probe, Fla-DNT, has been synthesized for the rapid and specific detection of H2S. Fla-DNT exhibits excellent selectivity and anti-interference properties, a short response time (4 min), large Stokes shift (138 nm), and low detection limit (1.357 µM). Upon exposure to H2S, Fla-DNT displays a remarkable increase in fluorescence intensity at 542 nm. Meanwhile, the recognizing site of H2S was predicted through Electrostatic potential and ADCH charges calculations, while the sensing mechanism of H2S was determined via HRMS analysis and DFT calculation. More importantly, the probe owes multiple applications, such as a recovery rate ranging from 92.00 to 102.10% for detecting H2S in water samples, and it can be fabricated into fluorescent strips to track H2S production during food spoilage by tracking color changes, thereby enabling real-time monitoring of food freshness. The bioimaging experiments demonstrate the capability of Fla-DNT to detect both endogenous and exogenous H2S in living cells. These results provide a reliable method and idea for H2S detection in complex environments.

Multiple Applications of a Novel Fluorescence Probe with Large Stokes Shift and Sensitivity for Rapid H2S Detection.

Herein, a novel fluorescence probe Fla-DNP based on flavonol has been designed and synthesized for rapid, specific detection of H2S. With the addition of H2S, Fla-DNP triggered thiolysis and released Fla displaying the "turn-on" fluorescence response at 566 nm, which is consistent with the reaction site predicted by calculating Electrostatic potential and ADCH charges. As an easily available H2S probe, Fla-DNP has the advantages of high selectivity, anti-interference, low detection limit (0.834 µM), short response time (6 min), and large Stokes shift (124 nm). The sensing mechanism of H2S was determined by HRMS analysis and DFT calculation. Moreover, Fla-DNP processes a wide range of multiple applications, including the detection of H2S in environmental water samples with good recovery rates ranging from 89.6% to 102.0%, as well as tracking the production of H2S during food spoilage. Meanwhile, the probe exhibits superior biocompatibility and can not only be available used for H2S detection in living cells but be further designed as an H2S-activated CO photoreleaser, based on which it can be developed as a targeted anti-cancer drug. A novel fluorescence probe Fla-DNP was synthesized utilizing 4-dimethylaminobenzoxanthone fluorescent dye (Fla) as the fluorophore, 2, 4-dinitrobenzenether group (DNP) as the recognition group, which can rapidly respond to H2S with high selectivity, anti-interference, low detection limit (0.834 µM), short response time (6 min), and large Stokes shift (124 nm) characteristics. The practical applications of Fla-DNP were further explored in water, foodstuffs samples and living cells. It is reflected that Fla-DNP can not only track H2S in complex environment water, but also can detect H2S produced during foodstuffs spoilage to monitor food freshness. More importantly, Fla-DNP can be available used for H2S detection in living cells and utilize the properties of the photoinduced release of CO from flavonols to be designed as a bifunctional platform for H2S detection and CO release. It is demonstrated that H2S-activated CO photoreleaser Fla-DNP has promise for development as an anti-cancer drug.

Counterion-Controlled Formation of Layered Honeycomb and Polythreading Uranyl Networks and the Highly Sensitive and Selective Detection of Fe3+ in Aqueous Media.

Under hydrothermal conditions, six uranium coordination polymers were obtained by employing the ligand of tris(2-carboxyethyl) isocyanurate (H3tci) and different combinations of d-block metal ions (Mn2+, Co2+, Zn2+, Ni2+) or N-donors (triethylamine (Et3N), 2,2'-bipyridine (2,2'-bipy)). Three uranium polymers [(UO2)2(tci)2]1/2-·[Mn2(µ2-O)(H2O)8]1/2+·2H2O (1), [(UO2)2(tci)2]1/2-·[Co2(µ2-O)(H2O)8]1/2+ (2), and [(UO2)2(tci)2]1/2-·[Zn2(µ2-O)(H2O)8]1/2+·2H2O (3) containing transition metal hydrated ions, crystallized as two-dimensional coordination polymers with the common (6, 3) net topology. X-ray crystal structures of 1-3 display that they have similar honeycomb-like frameworks with all ligands bis-chelating. [UO2(tci)]-3·[Ni(H2O)6]2+(H3O)+·2H2O (4) and [UO2(tci)]-·[NH(CH2CH3)3]1/3+·(2H3O+)1/3 (5) are made up of four interlocked sets and exhibit the 4-fold-interpenetrated frameworks. [UO2(tci)]-·(C10H9N2)+·H2O (6) comprises the 2,2'-bipy cation as counterion and represents a 2D grid layered structure. Additional metals and the N-donors are all free in the complexes, acting as the templates and compensation of the charge equilibrium. The solid-state emission spectra indicate that all of the synthesized compounds own fluorescence emissions. Furthermore, the results of the quenching ability of Fe3+ for complexes 5 and 6 exhibit their highly sensitive and selective detection for Fe3+ ions. Moreover, the uranium complexes can be used as a potential probe for Fe3+ in aqueous solutions.

Preparation of mesoporous Cs-POM@MOF-199@MCM-41 under two different synthetic methods for a highly oxidesulfurization of dibenzothiophene.

Two different synthetic methods, the direct method and the substitution method, were used to synthesize the Cs-POM@MOF-199@MCM-41 (Cs-PMM), in which the modified heteropolyacid with cesium salt has been encapsulated into the pores with the mixture of MOF and MCM-41. The structural properties of the as-prepared catalysts were characterized using various analytical techniques: powder X-ray diffraction, FT-IR, SEM, TEM, XPS and BET, confirming that the Cs-POM active species retained its Keggin structure after immobilization. The substitution method of Cs-PMM exhibited more excellent catalytic performance for oxidative desulfurization of dibenzothiophene in the presence of oxygen. Under optimal conditions, the DBT conversion rate reached up to 99.6% and could be recycled 10 times without significant loss of catalytic activity, which is mainly attributed to the slow leaching of the active heteropolyacid species from the strong fixed effect of the mixture porous materials.