Latest ArticlesA novel amine-modified pillar[5]arene bonded porous silica adsorbent (DETA-P5S) was designed to be applied to dynamic CO2 adsorption and selective separation of CO2 over N2 and CH4 gases mixture. The results demonstrated that reasonable introduction of DETA into the BE-P5 bonded silica support has significantly increased the adsorption capacity of CO2. The DETA-P5S has the optimal adsorption capacity of 9.1 mmol/g with 5 vol% CO2 at 40 ℃. The main reason of this increased capacity could be attributed to the enhanced CO2 diffusion into porous adsorbent for its better dispersion in the pores of amine-pillar[5]arene cavity and active site of DETA. Furthermore, the dynamic saturation adsorption capacities of DETA-P5S were 7.11 (0.37) and 6.18 (0.44) mmol/g for CO2/N2 and CO2/CH4, respectively, both the gas mixtures showed high separation selectivity. Simultaneously, the DETA-P5S can maintain outstanding CO2 adsorption capacity after fifteen regeneration cycles. Consequently, the designed DETA-P5S could serve as a promising adsorbent for CO2 capture and storage.
Small peptides have attracted increasing attention for their unique features and diverse biological functions. Achieving rapid separation and accurate quantification, however, remains a challenge because of their low abundance and the co-existence of numerous structural isomers. In this study, we developed a novel approach using isotope chemical labeling for ultrasensitive determination of di/tripeptides in biological samples. We successfully synthesized a novel derivatization reagent, 4-(2-(ethoxymethylene)-3-oxobutanamido)-N,N,N-trimethylbenzenaminium iodide (EOTMBA) as well as its deuterium-labeled isotope reagent (d3-EOTMBA). A total of 97 small peptides, including 89 dipeptides and 8 tripeptides, could be completely derivatized in methanol within 1.5 h at 60 ℃. After EOTMBA labeling, analysis of these di/tripeptides were achieved within 22 min by LC-MS/MS analysis. The method demonstrated 86.3%–113% accuracy and the limit of quantification ranged from 0.25 fmol/L to 5 nmol/L. Using this method, we achieved ultrasensitive and accurate quantification of di/tripeptides in 147 plasma, 49 urine and 46 bile samples obtained from healthy individuals and patients with biliary tract diseases. The identified differential di/tripeptide biomarker panels showed promising diagnostic performance for patients with biliary tract cancer with area under the receiver operating curve values from 0.870 to 0.996. Furthermore, this method was successfully applied to quantify di/tripeptides in the extract of an animal-derived traditional Chinese medicine, Eupolyphaga sinensis Walker. These findings highlight the possible application of the analytical method in clinics and for the purposes of quality control of traditional Chinese medicines.
The construction of enzyme reactors based on metal-organic frameworks (MOFs) as the immobilized matrix is a proven strategy that has achieved the widespread application of enzymes across industries. Although many MOFs and a variety of strategies have been developed, a formidable challenge remains in maintaining the high enzyme activity with excellent recyclability and tolerance for harsh conditions. Herein, using degradable redox stimuli-responsive liposomes as the templates with microporous MOFs (M-MOFs) as the hosts for enzyme encapsulation, a series of enzyme reactors (enzyme@M-MOFs) was designed and created. Based on the premise of enhancing enzyme protection in the harsh environment, this strategy provided a high degree-of-freedom space via removal of liposomes that improved the conformational freedom of the enzymes, promoted the mass transfer of substrates and products, and greatly boosted the catalytic activity. Importantly, the strategy had good universality and was applied to various liposomes, M-MOFs and enzymes. Additionally, the co-encapsulation of different enzymes with synergistic functions was performed using the M-MOFs platform. This study solved the problems of the conformation limitation of enzymes and mass transfer resistance of substrates and products using the proposed enzyme@M-MOFs, providing a new approach for the construction of biological cascade reaction devices based on MOFs materials.
The device configuration with mesoporous titanium dioxide (m-TiO2) has garnered considerable attention as a promising solution for high-stable perovskite and dye-sensitized solar cells, although its application in organic solar cells remains unexplored. In this communication, we have incorporated this structure into both bulk-heterojunction (BHJ) and single-component organic solar cells (SCOSCs). Surprisingly, mesoporous OSCs (M-OSCs) demonstrate a deteriorative efficiency in BHJ-type cells, whereas this configuration succeeds in SCOSCs, exhibiting competitive performance with planar OSCs (P-OSCs). This pioneering study has resulted in a competitive power conversion efficiency of 9.67% for m-TiO2-based cells, marking a significant milestone in the advancement of OSCs. Importantly, profiting from the better ultraviolet resistance of m-TiO2 than zinc oxide, this M-OSC exhibits superior photostability than that of P-OSCs when subjected to continuous one-sun (AM1.5G) illumination. In its entirety, this research not only introduces the concept of M-OSCs for the first time but also unveils a novel device architecture poised to address the long-term stability concerns within the realm of OSCs.
Gas adsorption remains an attractive area of research. The hierarchical structure can reduce diffusion limitations and facilitate molecular transport, while acid sites can be used as adsorption sites. These make zeolites widely used in the field of gas adsorption. How to obtain zeolite adsorbents with better adsorption properties by modulating the hierarchical structure and acid sites is a pressing issue nowadays. This review highlights the strategies to modulate the hierarchical structure as well as the acid sites; and then explains how these strategies are achieved. The mechanism of zeolite adsorption on gases is then described in terms of these two properties. Lastly, the adsorption properties of zeolites for certain gases under specific conditions are summarised. An outlook of zeolite hierarchical structures and acid site modulation strategies is given.
Benzo[4,5]imidazo[1,2-a]pyrimidine-based derivatives play crucial roles in medicines, pesticides, tracers and photoelectric materials. However, their synthesis approach still needs to be optimized, and their fluorescent properties in intracellular microenvironment are unclear. Here, a Cu(Ⅱ)-catalyzed cascade coupling cyclization reaction was successfully developed to synthesize benzo[4,5]imidazo[1,2-a]pyrimidine scaffold with mild reaction conditions, broad substrate scopes and high yields. After a system study, we found that compound 4aa displayed an optimal viscosity-specific response with remarkable fluorescence enhancement (102-fold) for glycerol at 490 nm. Particularly, 4aa possessed excellent structure-inherent targeting (SIT) capability for lysosome (P = 0.95) with high pH stability and large Stokes shift. Importantly, 4aa was validated for its effectiveness in diagnosing lysosomal storage disorders (LSD) in living cells. The 4aa also showed its potential to map the micro-viscosity and its metabolism process in zebrafish. This work not only affords an efficient protocol to fabricate benzo[4,5]imidazo[1,2-a]pyrimidine derivatives, reveals this skeleton has excellent SIT features for lysosome, but also manifests that 4aa can serve as a practical tool to monitor lysosomal viscosity and diagnose LSD.
Rechargeable magnesium ion batteries (RMBs) are investigated as lithium-ion batteries (LIBs) alternatives owing to their favorable merits of high energy density, abundance and low expenditure of Mg, as well as especially non-toxic safety and low risk of dendrite formation in anodes, which endows them to be more easily assembled in electric-power vehicles for the extended application of civilian-military fields. Nevertheless, the high charge density, strong polarization effect, and slow diffusion kinetics of Mg2+ remain a large obstacle and thus enormous efforts have to be paid to mend the gap with commercial demand for cathode materials. At present, RMBs cathode materials mainly contain transition metal sulfides/oxides, polyanionic compounds and Prussian blue analogs, and several methods such as nano structuring, doping regulation and coating modification have been applied to materials design for better performance. In this paper, the current research status of RMBs cathode materials at home & abroad is arranged and summarized along with challenges of development in the future focusing on synthesis of RMBs cathode materials with high energy density as well as satisfactory cycling performance. And this analysis aims to provide reference and basis for researchers working on RMBs technology advancement.
The electrocatalytic reduction of nitrate (NO3–) not only facilitates the environmentally sustainable production of ammonia (NH3) but also purifies water by removing NO3–, thereby transforming waste into valuable resources. The process of converting NO3– to NH3 is complex, involving eight electron transfers and multiple intermediates, making the choice of electrocatalyst critical. In this study, we report a cobalt selenide (CoSe2) nanowire array on carbon cloth (CoSe2/CC) as an effective electrocatalyst for the NO3– to NH3 conversion. In an alkaline medium with 0.1 mol/L NO3–, CoSe2/CC demonstrates exceptional NH3 Faradaic efficiency of 97.6% and a high NH3 yield of 517.7 µmol h–1 cm–2 at –0.6 V versus the reversible hydrogen electrode. Furthermore, insights into the reaction mechanism of CoSe2 in the electrocatalytic NO3– reduction are elucidated through density functional theory calculations.
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