Biomimetic Catalysis of a Porous Iron-Based Metal–Metalloporphyrin Framework

A porous metal–metalloporphyrin framework, MMPF-6, based upon an iron­(III)-metalated porphyrin ligand and a secondary binding unit of a zirconium oxide cluster was constructed; MMPF-6 demonstrated interesting peroxidase activity comparable to that of the heme protein myoglobin as well as exhibited solvent adaptability of retaining the peroxidase activity in an organic solvent

Fragment-Based Identification of Influenza Endonuclease Inhibitors

The influenza virus is responsible for millions of cases of severe illness annually. Yearly variance in the effectiveness of vaccination, coupled with emerging drug resistance, necessitates the development of new drugs to treat influenza infections. One attractive target is the RNA-dependent RNA polymerase PA subunit. Herein we report the development of inhibitors of influenza PA endonuclease derived from lead compounds identified from a metal-binding pharmacophore (MBP) library screen. Pyromeconic acid and derivatives thereof were found to be potent inhibitors of endonuclease. Guided by modeling and previously reported structural data, several sublibraries of molecules were elaborated from the MBP hits. Structure–activity relationships were established, and more potent molecules were designed and synthesized using fragment growth and fragment merging strategies. This approach ultimately resulted in the development of a lead compound with an IC₅₀ value of 14 nM, which displayed an EC₅₀ value of 2.1 μM against H1N1 influenza virus in MDCK cells

Self-Assembly of Oleyl Bis(2-hydroxyethyl)methyl Ammonium Bromide with Sodium Dodecyl Sulfate and Their Interactions with Zein

Surface tension and aggregation behavior in an aqueous solution of the mixture of cationic surfactant oleyl bis­(2-hydroxyethyl)­methylammonium bromide (OHAB) and anionic surfactant sodium dodecyl sulfate (SDS) have been studied by surface tension, conductivity, turbidity, zeta potential, isothermal titration microcalorimetry (ITC), cryogenic transmission electron microscopy (Cryo-TEM), and dynamic light scattering. The mixture shows pretty low critical micellar concentration and surface tension, and successively forms globular micelles, unilamellar vesicles, multilamellar vesicles, rod-like micelles, and globular micelles again by increasing the molar fraction of OHAB from 0 to 1.00. The cooperation of hydrophobic interaction between the alkyl chains, electrostatic attraction between the headgroups as well as hydrogen bonds between the hydroxyethyl groups leads to the abundant aggregation behaviors. Furthermore, the solubilization of zein by the OHAB/SDS aggregates and their interactions were studied by ITC, total organic carbon analysis (TOC), and Cryo-TEM. Compared with pure OHAB or pure SDS solution, the amount of zein solubilized by the OHAB/SDS mixture is significantly reduced. It means that the mixtures have much stronger abilities in solubilizing zein. This result has also been proved by the observed enthalpy changes for the interaction of OHAB/SDS mixture with zein. Mixing oppositely charged OHAB and SDS reduces the net charge of mixed aggregates, and thus, the electrostatic attraction between the aggregates and zein is weakened. Meanwhile, the large size of the aggregates may increase the steric repulsion to the zein backbone. This work reveals that surfactant mixtures with larger aggregates and smaller CMCs solubilize less zein, suggesting how to construct a highly efficient and nonirritant surfactant system for practical use

Image_3_Microbial community and soil enzyme activities driving microbial metabolic efficiency patterns in riparian soils of the Three Gorges Reservoir.JPEG

Riparian zones represent important transitional areas between aquatic and terrestrial ecosystems. Microbial metabolic efficiency and soil enzyme activities are important indicators of carbon cycling in the riparian zones. However, how soil properties and microbial communities regulate the microbial metabolic efficiency in these critical zones remains unclear. Thus, microbial taxa, enzyme activities, and metabolic efficiency were conducted in the riparian zones of the Three Gorges Reservoir (TGR). Microbial carbon use efficiency and microbial biomass carbon had a significant increasing trend along the TGR (from upstream to downstream); indicating higher carbon stock in the downstream, microbial metabolic quotient (qCO2) showed the opposite trend. Microbial community and co-occurrence network analysis revealed that although bacterial and fungal communities showed significant differences in composition, this phenomenon was not found in the number of major modules. Soil enzyme activities were significant predictors of microbial metabolic efficiency along the different riparian zones of the TGR and were significantly influenced by microbial α-diversity. The bacterial taxa Desulfobacterota, Nitrospirota and the fungal taxa Calcarisporiellomycota, Rozellomycota showed a significant positive correlation with qCO2. The shifts in key microbial taxa unclassified_k_Fungi in the fungi module #3 are highlighted as essential factors regulating the microbial metabolic efficiency. Structural equation modeling results also revealed that soil enzyme activities had a highly significant negative effect on microbial metabolism efficiency (bacteria, path coefficient = −0.63; fungi, path coefficient = −0.67).This work has an important impact on the prediction of carbon cycling in aquatic-terrestrial ecotones.Graphical abstract</p

Mimic Carbonic Anhydrase Using Metal–Organic Frameworks for CO₂ Capture and Conversion

Carbonic anhydrase (CA) is a zinc-containing metalloprotein, in which the Zn active center plays the key role to transform CO₂ into carbonate. Inspired by nature, herein we used metal–organic frameworks (MOFs) to mimic CA for CO₂ conversion, on the basis of the structural similarity between the Zn coordination in MOFs and CA active center. The biomimetic activity of MOFs was investigated by detecting the hydrolysis of <i>para</i>-nitrophenyl acetate, which is a model reaction used to evaluate CA activity. The biomimetic materials (e.g., CFA-1) showed good catalytic activity, and excellent reusability, and solvent and thermal stability, which is very important for practical applications. In addition, ZIF-100 and CFA-1 were used to mimic CA to convert CO₂ gas, and exhibited good efficiency on CO₂ conversion compared with those of other porous materials (e.g., MCM-41, active carbon). This biomimetic study revealed a novel CO₂ treatment method. Instead of simply using MOFs to absorb CO₂, ZIF-100 and CFA-1 were used to mimic CA for in situ CO₂ conversion, which provides a new prospect in the biological and industrial applications of MOFs

Immobilizing Highly Catalytically Active Noble Metal Nanoparticles on Reduced Graphene Oxide: A Non-Noble Metal Sacrificial Approach

In this work, we have developed a non-noble metal sacrificial approach for the first time to successfully immobilize highly dispersed AgPd nanoparticles on reduced graphene oxide (RGO). The Co₃(BO₃)₂ co-precipitated with AgPd nanoparticles and subsequently sacrificed by acid etching effectively prevents the primary AgPd particles from aggregation. The resulted ultrafine AgPd nanoparticles exhibit the highest activity (turnover frequency, 2739 h^–1 at 323 K) among all the heterogeneous catalysts for the dehydrogenation of formic acid to generate hydrogen without CO impurity. The sacrificial approach opens up a new avenue for the development of high-performance metal nanocatalysts

Generalized Ratiometric Indicator Based Surface-Enhanced Raman Spectroscopy for the Detection of Cd²⁺ in Environmental Water Samples

The concept of generalized ratiometric indicator based surface-enhanced Raman spectroscopy was first introduced and successfully implemented in the detection of Cd²⁺ in environmental water samples using Au nanoparticles (AuNPs) modified by trithiocyanuric acid (TMT). Without the use of any internal standard, the proposed method achieved accurate concentration predictions for Cd²⁺ in environmental water samples with recoveries in the ranges of 91.8–108.1%, comparable to the corresponding values obtained by atomic absorption spectroscopy. The limit of detection and limit of quantification were estimated to be 2.9 and 8.7 nM, respectively. More importantly, other species present in water samples which cannot react with TMT and have weaker binding ability to AuNPs than TMT do not interfere with the quantification of Cd²⁺. Therefore, it is expected that the combination of the generalized ratiometric indicator based surface-enhanced Raman spectroscopy with the proposed AuNP–TMT probing system can be a competitive alternative for the primary screening of Cd²⁺ pollution

Image_2_Microbial community and soil enzyme activities driving microbial metabolic efficiency patterns in riparian soils of the Three Gorges Reservoir.jpg

Riparian zones represent important transitional areas between aquatic and terrestrial ecosystems. Microbial metabolic efficiency and soil enzyme activities are important indicators of carbon cycling in the riparian zones. However, how soil properties and microbial communities regulate the microbial metabolic efficiency in these critical zones remains unclear. Thus, microbial taxa, enzyme activities, and metabolic efficiency were conducted in the riparian zones of the Three Gorges Reservoir (TGR). Microbial carbon use efficiency and microbial biomass carbon had a significant increasing trend along the TGR (from upstream to downstream); indicating higher carbon stock in the downstream, microbial metabolic quotient (qCO2) showed the opposite trend. Microbial community and co-occurrence network analysis revealed that although bacterial and fungal communities showed significant differences in composition, this phenomenon was not found in the number of major modules. Soil enzyme activities were significant predictors of microbial metabolic efficiency along the different riparian zones of the TGR and were significantly influenced by microbial α-diversity. The bacterial taxa Desulfobacterota, Nitrospirota and the fungal taxa Calcarisporiellomycota, Rozellomycota showed a significant positive correlation with qCO2. The shifts in key microbial taxa unclassified_k_Fungi in the fungi module #3 are highlighted as essential factors regulating the microbial metabolic efficiency. Structural equation modeling results also revealed that soil enzyme activities had a highly significant negative effect on microbial metabolism efficiency (bacteria, path coefficient = −0.63; fungi, path coefficient = −0.67).This work has an important impact on the prediction of carbon cycling in aquatic-terrestrial ecotones.Graphical abstract</p

Image_1_Microbial community and soil enzyme activities driving microbial metabolic efficiency patterns in riparian soils of the Three Gorges Reservoir.JPEG

Riparian zones represent important transitional areas between aquatic and terrestrial ecosystems. Microbial metabolic efficiency and soil enzyme activities are important indicators of carbon cycling in the riparian zones. However, how soil properties and microbial communities regulate the microbial metabolic efficiency in these critical zones remains unclear. Thus, microbial taxa, enzyme activities, and metabolic efficiency were conducted in the riparian zones of the Three Gorges Reservoir (TGR). Microbial carbon use efficiency and microbial biomass carbon had a significant increasing trend along the TGR (from upstream to downstream); indicating higher carbon stock in the downstream, microbial metabolic quotient (qCO2) showed the opposite trend. Microbial community and co-occurrence network analysis revealed that although bacterial and fungal communities showed significant differences in composition, this phenomenon was not found in the number of major modules. Soil enzyme activities were significant predictors of microbial metabolic efficiency along the different riparian zones of the TGR and were significantly influenced by microbial α-diversity. The bacterial taxa Desulfobacterota, Nitrospirota and the fungal taxa Calcarisporiellomycota, Rozellomycota showed a significant positive correlation with qCO2. The shifts in key microbial taxa unclassified_k_Fungi in the fungi module #3 are highlighted as essential factors regulating the microbial metabolic efficiency. Structural equation modeling results also revealed that soil enzyme activities had a highly significant negative effect on microbial metabolism efficiency (bacteria, path coefficient = −0.63; fungi, path coefficient = −0.67).This work has an important impact on the prediction of carbon cycling in aquatic-terrestrial ecotones.Graphical abstract</p

Image_6_Microbial community and soil enzyme activities driving microbial metabolic efficiency patterns in riparian soils of the Three Gorges Reservoir.JPEG

Riparian zones represent important transitional areas between aquatic and terrestrial ecosystems. Microbial metabolic efficiency and soil enzyme activities are important indicators of carbon cycling in the riparian zones. However, how soil properties and microbial communities regulate the microbial metabolic efficiency in these critical zones remains unclear. Thus, microbial taxa, enzyme activities, and metabolic efficiency were conducted in the riparian zones of the Three Gorges Reservoir (TGR). Microbial carbon use efficiency and microbial biomass carbon had a significant increasing trend along the TGR (from upstream to downstream); indicating higher carbon stock in the downstream, microbial metabolic quotient (qCO2) showed the opposite trend. Microbial community and co-occurrence network analysis revealed that although bacterial and fungal communities showed significant differences in composition, this phenomenon was not found in the number of major modules. Soil enzyme activities were significant predictors of microbial metabolic efficiency along the different riparian zones of the TGR and were significantly influenced by microbial α-diversity. The bacterial taxa Desulfobacterota, Nitrospirota and the fungal taxa Calcarisporiellomycota, Rozellomycota showed a significant positive correlation with qCO2. The shifts in key microbial taxa unclassified_k_Fungi in the fungi module #3 are highlighted as essential factors regulating the microbial metabolic efficiency. Structural equation modeling results also revealed that soil enzyme activities had a highly significant negative effect on microbial metabolism efficiency (bacteria, path coefficient = −0.63; fungi, path coefficient = −0.67).This work has an important impact on the prediction of carbon cycling in aquatic-terrestrial ecotones.Graphical abstract</p