Quality Evaluation of Metabolic-Associated Fatty Liver Disease Guidelines and Expert Consensus.

The purpose of this study is to evaluate and analyze the quality of guidelines and expert consensus on clinical practice regarding metabolically associated fatty liver disease (MAFLD) over the past five years. Data from the websites were retrieved using computers. We evaluated guidelines and expert consensus on MAFLD that were officially published between January 1, 2018 and March 24, 2023. Two evaluators independently examined the literature and extracted data. The included literature on guidelines and expert consensus was then subjected to quality review and analysis using assessment tools from Appraisal of Guidelines for Research and Evaluation (AGREE) II and the Joanna Briggs Institute Qualitative Assessment and Review Instrument (JBI-QARI) (2016). The intraclass correlation coefficient (ICC) values of all items on the AGREE II scale for the two evaluators were greater than 0.75, indicating a high degree of agreement between their assessments. Scope and purpose (48.90%), participants (49.21%), rigor in the formulation process (56.97%), clarity of expression (90.08%), applicability (66.08%), and independence of file compiling (60.12%) were the AGREE II scoring items with the standardized average scores. Apart from the participants, the average scores of all the scoring items in the guidelines from other countries other than China were higher than those from China (|Z|+>+2.272, p+<+0.05). MAFLD guidelines must be revised to enhance their methodological quality. When creating guidelines, it is recommended that the formulators strictly adhere to the formulation and drafting standards of AGREE II and elevate the quality of the guidelines.

Scalable Palladium-Catalyzed Alkoxycarbonylation of Conjugated Dienes.

The Pd(cod)Cl2-catalyzed alkoxycarbonylation of conjugated dienes to ß,γ-unsaturated esters was approached by both intramolecular phosphinesulfonate L1 and intermolecular PPh3/PTSA in this study. However, the poor solubility of the Pd/L1 complex and the labile monodentate Pd/PPh3 structure restricts the system efficiency, especially for the scale-up application. By contrast, the stable and well-soluble bidentate Xantphos system allows for the quantitative formation of 3-pentenoate (96%) on a gram scale within 6 h in weakly alkaline N-methylpyrrolidone (NMP), which also functions as a basic site to promote the rate-limiting alcoholysis step while reducing the dosage of ligand to a theoretical value.

Observation of a bcc-like framework in polyhydrido copper nanoclusters.

Cu is well-known to adopt a face-centered cubic (fcc) structure in the bulk phase. Ligand-stabilized Cu nanoclusters (NCs) with atomically precise structures are an emerging class of nanomaterials. However, it remains a great challenge to have non-fcc structured Cu NCs. In this contribution, we report the syntheses and total structure determination of six 28-nuclearity polyhydrido Cu NCs: [Cu28H16(dppp)4(RS)4(CF3CO2)8] (dppp = 1,3-bis(diphenylphosphino)propane, RSH = cyclohexylthiol, 1; tert-butylthiol, 3; and 2-thiophenethiol, 4) and [Cu28H16(dppe)4(RS)4(CH3CO2)6Cl2] (dppe = 1,2-bis(diphenylphosphino)ethane, RSH = (4-isopropyl)thiophenol, 2; 4-tert-butylbenzenethiol, 5; and 4-tert-butylbenzylmercaptan, 6). Their well-defined structures solved by X-ray single crystal diffraction reveal that these 28-Cu NCs are isostructural, and the overall metal framework is arranged as a sandwich structure with a core-shell Cu2@Cu16 unit held by two Cu5 fragments. One significant finding is that the organization of 18 Cu atoms in the Cu2@Cu16 could be regarded as an incomplete and distorted version of 3 × 2 × 2 "cutout" of the body-centered cubic (bcc) bulk phase, which was strikingly different to the fcc structure of bulk Cu. The bcc framework came as a surprise, as no bcc structures have been previously observed in Cu NCs. A comparison with the ideal bcc arrangement of 18 Cu atoms in the bcc lattice suggests that the distortion of the bcc structure results from the insertion of interstitial hydrides. The existence, number, and location of hydrides in these polyhydrido Cu NCs are established by combined experimental and DFT results. These results have significant implications for the development of high-nuclearity Cu hydride NCs with a non-fcc architecture.

Ionic framework constructed with protic ionic liquid units for improving ammonia uptake.

In this work, an ionic framework [Ph3ImH][Tf2N]2 constructed from protic imidazolium ionic liquid units through ionic and hydrogen bonding interactions was synthesized for selective ammonia uptake. Investigation of the NH3 uptake mechanism indicates that the acid sites in [Ph3ImH][Tf2N]2 would be frustrated when contacted with NH3, and the frustration of [Ph3ImH][Tf2N]2 precipitates NH3 capture by hydrogen bonding and physical interactions, and the NH3 could be released under mild conditions. There was no obvious decrease in capacity over 10 consecutive cycles of ammonia uptake and release.

Immobilization of ß-1,3-xylanase on pitch-based hyper-crosslinked polymers loaded with Ni2+ for algal biomass manipulation.

ß-1,3-xylanase plays an important role in the conversion of algal biomass into renewable chemical commodities and functional xylooligosaccharides. Efficient immobilization of the target enzymes that could integrate the separation, purification, and immobilization in one-step may have great potentials. The cheap and easily obtained pitch was adopted as the raw material to prepare the hyper-cross-linked polymers with the specific surface areas of 560 m2/g and the Ni2+ loading about 80 mg/g. As a carrier, it could immobilize and purify the ß-1,3-xylanases directly from the crude cell debris with the activity recovery of (80.66 ± 0.87) %. The half-life of the immobilized ß-1,3-xylanases was 50 min at 50 °C, which was significantly longer than the free ones with only 14 min. The immobilized ß-1,3-xylanases could retain 65 % of the activity after stored at 30 ℃ for 80 h, they could also retain 87 % of the original activity after 15 cycles of reuse. In terms of potential applications in the manipulation of algae Caulerpa lentillifera, the immobilized ß-1,3-xylanases could release 30 % more reducing sugar in 85 h. The method proposed here is promising for algal biomass manipulation because of its low cost, stable storage, convenient recycling and excellent reusability.

A Sodalite-Type Silver Orthophosphate Cluster in a Globular Silver Nanocluster.

The synthesis and structure of a giant 102-silver-atom nanocluster (NC) 1 is presented. X-ray structural analysis reveals that 1 features a multi-shelled metallic core of Ag6 @Ag24 @Ag60 @Ag12 . An octahedral Ag6 core is encaged by a truncated octahedral Ag24 shell. The Ag24 shell is composed of a hitherto unknown sodalite-type silver orthophosphate cluster (SOC) {(Ag3 PO4 )8 }, reminiscent of the Ag3 PO4 photocatalyst. The SOC is capped by six interstitial sulfur atoms, giving a unique anionic cluster [Ag6 @{(Ag3 PO4 )8 }S6 ]6- , which functions as an intricate polyhedral template with abundant surface O and S atoms guiding the formation of a rare rhombicosidodecahedral Ag60 shell. An array of 6 linear Ag2 staples further surround this Ag60 shell. [Ag6 @{(Ag3 PO4 )8 }S6 ]6- is an unusual Ag-based templating anion to induce the assembly of a SOC within silver NC. This finding provides molecular models for bulk Ag3 PO4 , and offers a fresh template strategy for the synthesis of silver NCs with high symmetry.

New protective ligands for atomically precise silver nanoclusters.

Atomically precise silver nanoclusters (NCs) have emerged as a hot topic attracting immense research interest. Protecting ligands are needed for direct capping on cluster surfaces in order to prevent aggregation and to stabilize NCs. It has been demonstrated that protective ligands are critical to determining the sizes, structures and properties of silver NCs. The past decades have witnessed conventionally used organic ligands (thiolates/selenols, phosphines and alkynyls) and inorganic ligands (chalcogens and halogens) being extensively used to passivate NC surfaces. However, only in the most recent years have new-type protecting ligands beyond the conventional ones begun to be introduced in the protecting sphere of new functional silver NCs. The present Frontier article covers the most recent examples of some new protective agents for well-defined silver NCs. We describe four classes of novel silver NCs stabilized by newly-developed surface ligands, namely, nitrogen-donor organic ligands, oxygen-donor inorganic ligands, metalloligands and macrocyclic hosts, paying attention to the synthesis, structures and properties of these silver NCs. This Frontier article will hopefully attract more cluster scientists to explore more freshly ligated atomically precise silver NCs with novel structures and properties in the years ahead. The literature survey in this review is based on publications up to February 2020. Some suggestions for future directions in this field are also given.

Cooperative CO2 absorption by amino acid-based ionic liquids with balanced dual sites.

In this study, a variety of functionalized ILs with dual sites including amino acid group (AA) and basic anion (R) were synthesized to investigate the suppression and cooperation between the sites in CO2 absorption. The basic anions selected in this study with different basicity include sulfonate (Su), carboxylate (Ac), imidazolium (Im), and indolium (Ind). These ILs ([P66614]2[AA-R]) were applied to CO2 absorption. The results present that CO2 capacity increases first and then decreases later with the continuous increase in the activity of the anion site. Combined with CO2 absorption experiments, IR and NMR spectroscopic analyses and DFT calculation demonstrate that the ability of one site to capture CO2 would be suppressed when the activity of another site is much stronger. Thus, the cooperation of dual site-functionalized ILs and high CO2 capacity might be achieved through balancing the two sites to be equivalent. Based on this point, [P66614]2[5Am-iPA] was further synthesized by taking the advantage of the conjugated benzene ring. As expected, [P66614]2[5Am-iPA] showed capacity as high as 2.38 mol CO2 per mol IL at 30 °C and 1 bar without capacity decrease even after 10 times recycling performance of CO2 absorption and desorption.

Enhanced CO2 capture by reducing cation-anion interactions in hydroxyl-pyridine anion-based ionic liquids.

In this work, an efficient strategy for improving CO2 capture based on anion-functionalized ionic liquids (ILs) by reducing cation-anion interactions in ILs was reported. The influence of the cationic species on CO2 absorption was investigated using 2-hydroxyl pyridium anions ([2-Op]) as a probe. CO2 capture experiments indicated that the CO2 absorption capacity in [2-Op] anion-based ILs varied from 0.94 to 1.69 mol CO2 per mol IL at 30 °C and 1 atm. Spectroscopic analysis and quantum chemical calculations suggested that the increase of the CO2 absorption capacity may be ascribed to the reduction of the strength of cation-anion interactions in ILs, and stronger cation-anion interactions would make one CO2 site in the [2-Op] anion inactive. Furthermore, the effect of the cation unit on the anion was evidenced by FT-IR spectra, implying that strong interactions between ions may lead to the decrease of the IR absorption wavenumber of hydroxy pyridium and work against CO2 capture. Following this strategy, it was finally found that [Ph-C8eim][2-Op] (Ph-C8eim = 1-N-ethyl-3-N-octyl-2-phenylimidazolium) with weaker cation-anion interactions exhibited a significant increase in the CO2 uptake capacity, and extremely high capacities of 1.69 and 1.83 mol CO2 per mol IL could be achieved at 30 and 20 °C, respectively. The study presented here would be helpful for further designing novel and effective ILs for advancing CO2 capturing performance.

Tethered sensitizer-catalyst noble-metal-free molecular devices for solar-driven hydrogen generation.

Inspired by natural photosynthesis in an organized assembly, compact H2-evolving molecular devices, which tether sensitizer and catalyst modules in one single molecule, present an opportunity to overcome the diffusion limit required for multi-component molecular systems, and increase intramolecular electron transfer rates from the photoactivated unit to the catalytic center to improve H2-evolving efficiency. Thereinto absolutely noble-metal free H2-evolving molecular devices are of particular interest because they don't contain precious and scarce noble-metal based components. This Frontier article focuses specifically on the recent advances in the design, synthesis, and photocatalytic properties of all-abundant-element molecular devices for photoinduced H2 generation via intramolecular processes. Some challenges and suggestions for future directions in this field are also illustrated.

The Difference Se Makes: A Bio-Inspired Dppf-Supported Nickel Selenolate Complex Boosts Dihydrogen Evolution with High Oxygen Tolerance.

Inspired by the metal active sites of [NiFeSe]-hydrogenases, a dppf-supported nickel(II) selenolate complex (dppf=1,1'-bis(diphenylphosphino)ferrocene) shows high catalytic activity for electrochemical proton reduction with a remarkable enzyme-like H2 evolution turnover frequency (TOF) of 7838 s-1 under an Ar atmosphere, which markedly surpasses the activity of a dppf-supported nickel(II) thiolate analogue with a low TOF of 600 s-1 . A combined study of electrochemical experiments and DFT calculations shed light on the catalytic process, suggesting that selenium atom as a bio-inspired proton relay plays a key role in proton exchange and enhancing catalytic activity of H2 production. For the first time, this type of Ni selenolate-containing electrocatalyst displays a high degree of O2 and H2 tolerance. Our results should encourage the development of the design of highly efficient oxygen-tolerant Ni selenolate molecular catalysts.

Regulation of shrimp PjCaspase promoter activity by WSSV VP38 and VP41B.

Members of the Caspase family play essential roles in apoptosis. In kuruma shrimp Marsupenaeus japonicus the caspase gene (PjCaspase) was previously found dramatically up-regulated in viral-challenged and -resistant shrimp, suggesting that PjCaspase plays an important role in protecting host from viral infection. In order to further delineate the transcriptional regulation of PjCaspase in response to viral infection, the promoter activity was confirmed by fusing the 5'-flanking promoter region of the PjCaspase gene to the enhanced green fluorescence protein (EGFP) gene and transformed to Trichoplusia ni High Five™ cell line. With streptavidin-bead pulldown assay, two envelope proteins VP38 and VP41B of white spot syndrome virus (WSSV) were found to bind to PjCaspase promoter in vitro. Luciferase reporter assay by cotransfection of PjCaspace promoter with VP38 or VP41B revealed that the proteins act as repressor and activator of PjCaspase transcription respectively. Our study suggested a potential role for the two WSSV proteins on shrimp PjCaspase regulation in response to WSSV challenge. To our knowledge this is the first report on WSSV envelope proteins found to be involved in gene regulation. These results provide insights into the molecular regulation of PjCaspase gene expression, which will be helpful for shrimp viral disease control.