Wiley最新文献

ZnNb₂O₆ and a heterojunction ZnNb₂O₆/SnO₂ have been synthesized, characterized, and studied for its photocatalytic activity against organic and pharmaceutical pollutants under UV irradiation. The characterization techniques include X-ray Diffraction (XRD), ultraviolet-visible reflectance spectroscopy (UV–vis DRS), field emission scanning electron microscopy (FESEM), photoluminescence spectra (PL), and X-ray photoelectron spectroscopy (XPS). XRD confirms single phase formation. The particles sizes of ZnNb₂O₆ and ZnNb₂O₆/SnO₂ heterojunction are in range of 170–200 nm and 110–140 nm, respectively. Bandgaps as revealed by UV–vis DRS spectra are in the range 3.14–3.71 eV. The n-n type semiconductor heterojunction ZnNb₂O₆/SnO₂ shows enhanced photocatalytic activity than the individual components for degradation of pollutants due to more effective charge carrier separation. The rate of degradation by the heterojunction is twice that of the individual components. Methyl orange degradation pathways have been proposed using HRMS analysis. This is the first report of pharmaceutical antibiotic pollutants degradation by ZnNb₂O₆.

The remarkable properties of 2D nanomaterials are well known. However, their high interfacial adhesion energy often leads to restacking issues, limiting their potential in various applications. A strategic synthetic approach is presented to overcome this challenge. Specifically, the study first demonstrates the use of layered aluminosilicate as a sacrificial 2D template to allow the growth of highly ordered meso-holey polymeric layers, which can be subsequently exfoliated upon the removal of aluminosilicate and thermally converted to perpendicularly open meso-holey carbon (POMC). On the other hand, perpendicularly blocked meso-holey carbon (PBMC) is obtained with non-sacrificial 2D template of graphene oxide. When both POMC and PBMC are evaluated by operando hydrodynamic electrochemical impedance spectroscopy and transmission line model analysis for electrochemical reduction of oxygen, POMC achieves a remarkable improvement of charge transfer and mass transfer by up to 4.1 and 7.9 times, respectively, as compared to PBMC. This study therefore highlights the importance of perpendicularly open 2D nanoarchitectures in circumventing the restacking effect, offering valuable insights for leveraging 2D nanomaterials with open meso-holes in various applications.

Well-Tempered Metadynamics (WT-MetaD) simulations indicate that composite materials made up of Na-Montmorillonite (Na-MMT) coated with ionic liquids (ILs) having hydrophilic cations serve as good adsorbents for a hexameric (1,4) linked b-D-glucopyranoside (BGLC). Hydrophilic IL cations are effectively coated on the negative charges lining the Na-MMT surface while attracting simultaneously the polar oligosaccharides. In this work we have used two less conventional polyethylene glycol (PEG) based IL cations, [mim2 peg1]2+ and [mim2 peg2]2+, paired with [tf2N]- and Cl- anions. Another strongly hydrophilic ion combination, [C2OHmim][Cl], also showed great promise in effective oligosaccharide adsorption on the Na-MMT surface. The study reveals that the topological polar surface area (TPSA), the octanol-water partition coefficient (log PO/W), the length of the cationic side chain and the Debye screening length  of the IL are some of the most important factors affecting the adsorption of hydrophilic oligosaccharides on the clay-IL composites. Among all the systems studied, [mim2 peg2][tf2N]2 having the highest TPSA and a long screening length emerged as the best adsorbent of the oligosaccharide on the IL-coated clay.

The functional stay-green trait is a major goal of rice breeding. Here, we cloned OsSCE1a encoding SUMO-conjugating enzyme from Yuanjiang common wild rice, which simultaneously regulates the functional stay-green trait and growth duration. Low expression or knocking out OsSCE1a corresponded to increased chlorophyll content, photosynthetic competence, N use efficiency and a shortened growth period without affecting yield. A natural MITE-transposon insertion/deletion in the OsSCE1a promoter is the functional variation that regulates these traits. OsSCE1a was selected during evolution and shows significant variation between indica and japonica rice. OsNAC2 interacts with the MITE to enhance OsSCE1a expression. Genetic manipulation of OsSCE1a revealed its potential for rice improvement. OsSCE1a-mediated SUMOylation of OsGS2 suppresses GS (involved in N assimilation) enzyme activity. OsSCE1a also regulates growth duration by SUMOylating the transcription factor such as OsGBP1, which regulates the expression of the key heading gene Ghd7. Our findings shed light on the role of SUMOylation in crops and provide a strategy for increasing agricultural productivity.

Photocatalytic hydrogen peroxide and hydrogen production are the utmost encouraging ways to overcome the imminent energy catastrophe. For accomplishing these goals the photocatalysts needs to be stable, trap photons and superior exciton separation, yet these properties are scanty for Zr-MOFs. Hence, UiO-66-NH2 is armed with Carbon nanoparticles that were incorporated through facile solvothermal procedure are employed towards photocatalytic H2 and H2O2 production. Composite UC-2 exhibits an H2O2 generation rate of 33.2 μmol h-1 in an O2 saturated conditions with isopropyl alcohol and water underneath visible light irradiation. This H2O2 generation rate was nearly three folds higher than the pristine UiO-66-NH2 MOF. Moreover, the produced materials were subjected to a photocatalytic H2 evolution research, and similar results were obtained, indicating that UC-2 has the maximum H2 evolution capacity at 298.1 μmol h-1. The UC-2 composite exhibits improved photocatalytic activity, which was ascribed to the composites capacity to suppress exciton re-combination, enhanced photon capture and to facilitate quicker charge transfer. Typically, the light trapping tendency, remarkable electron transfer capacity and electron capture capacity of the carbon NPs based co-catalyst aids to improve the overall photo-reaction performance thereby producing superior photocatalytic H2O2 and H2 as a sustainable energy alternative.

Exploring heterojunction formation between conjugated organic polymer and metal-based semiconductors with promoted charge transfer and efficient spatial charge separation has proven to be quite successful in reinforcing photocatalytic wastewater treatment. Focusing on the removal of sulfonamide antibiotics from water, herein, we report BaTiO₃/I@g-C₃N₄ Z-scheme heterojunction photocatalyst for degradation of sulfamethazine (SMZ) pollutant. The optimized heterojunction 25ICN/BT exhibits superior 94.5% removal of SMZ in 90 min, which is nearly 11 and 5 times faster than BT and pristine I@g-C₃N₄ under visible light. The good repeatability of 25BT/ICN was proved by four-cycle experiments. The remarkable improvement in photocatalytic activity was due to effective Z-scheme transfer, diminished recombination, high charge transfer capacity, and redox capability. This was ascertained by electrochemical experiments and photoluminescence measurements. Furthermore, the degradation intermediates formed during the photocatalytic oxidation of SMZ were detected via liquid chromatography-mass spectrometry, and a suitable degradation pathway was suggested. The heterojunctions showed excellent performance in river, lake, and tap water and for other antibiotic pollutants. The radical quenching experiments and band structure analysis inferred ^•O₂⁻ radicals as main active species. This work lays down new perspectives on hierarchical heterostructures for the superior removal of noxious antibiotic contaminants.

Compositional Site Disorder Enables Engineering Oxide Phase Transitions

Work by Elliot J. Fuller and co-workers demonstrates that tunable disorder in a crystal can be quite useful: compositional site disorder was used to modify oxide semiconductors by changing the carrier type, improving crystallinity and tuning a spin transition. Applications include electrothermal thresholding devices such as radio frequency limiters. More details can be found in article number 2406885.

Background: Bilirubin is a by-product of haemoglobin breakdown and has been reported to be a potent antioxidant recently. While elevated levels of bilirubin have been linked to a reduced risk of various diseases, their role remains unknown in frailty. This study aims to explore the relationship between serum bilirubin levels and the risk of frailty.

Methods: This cohort study included 442 223 White British participants (aged 39 to 73 years) with an available frailty index at baseline (2006 to 2010) from the UK Biobank. The associations of total/direct bilirubin levels with the continuous frailty index were analysed by multivariable linear regression, and multivariable logistic regression was used after classifying frailty outcomes into non-frailty, pre-frailty and frailty. A Mendelian randomization (MR) analysis was applied to evaluate the association of genetically predicted bilirubin levels with frailty risk.

Results: The prevalence rates of both pre-frailty and frailty were 46.17% and 12.49%, respectively, with higher rates observed in women than in men (pre-frailty: 47.33% vs. 44.79%, frailty: 13.64% vs. 11.13%, respectively). There was a non-linear negative association between total bilirubin levels and frailty indexes (p < 0.0001). Mildly elevated total bilirubin levels had protective effects against pre-frailty (OR = 0.863, 95% CI: 0.849 to 0.879, p < 0.001) and frailty (OR = 0.660, 95% CI: 0.641 to 0.679, p < 0.001). Increased total bilirubin levels were more beneficial for women with frailty risk (percent changes per SD μmol/L = -0.37%, 95% CI: -0.40% to -0.34%). The MR analysis revealed a negative association between genetically predicted total/direct bilirubin levels and frailty risk (both p < 0.0001).

Conclusions: Circulating total/direct bilirubin levels were negatively associated with frailty risk in White British individuals. Mildly elevated total bilirubin levels were more beneficial for women subpopulation.

Signal drift and hysteresis of flexible piezoresistive sensors pose significant challenges against the widespread applications in emerging fields such as electronic skin, wearable equipment for metaverse and human-AI (artificial intelligence) interfaces. To address the creep and relaxation issues associated with pressure-sensitive materials, a highly stable piezoresistive composite is proposed, using polyamide-imide (PAI) fibers as the matrix and in situ grafted-polymerized polyaniline (PANI) as the semi-conducting layer. The PAI with large rigid fluorenylidene groups exhibits a high glass transition temperature of 372 °C (PAI 5-5), which results in an extremely long relaxation time at room temperature and consequently offers outstanding anti-creep/relaxation performances. The enhancement of PAI-PANI interfacial bonding through in situ grafting improves the sensor reliably. The sensor presents high linear sensitivity of 35.3 kPa^-1 over a pressure range of 0.2-20 kPa, outstanding repeatability, and excellent dynamic stability with only a 3.8% signal deviation through ≈10 000 cycles. Real-time visualization of pressure distribution is realized by sensor matrices, which demonstrate the capability of tactile gesture recognition on both flat and curved surfaces. The recognition of sitting postures is achieved by two 12 × 12 matrices facilitated by machine learning, which prompts the potential for the augmentation of smart driving.

Dicyanomethylene-terminated quinoidal materials are promising n-type organic semiconductors featuring excellent electron mobilities and air stability. Traditional synthetic methods of these materials such as Takahashi reaction, require the use of expensive palladium catalyst and halogenated substrates. However, for electron-rich fused aromatic compounds, the poor stability after halogenation renders their halogenated derivatives unsuitable as reaction precursors. To address this issue, we present a new metal-free synthetic approach using 2-(dimethylsulfaneylidene)malononitrile as the quinoidization reagent, which is successfully applied to various electron-rich fused aromatic compounds, leading to the corresponding quinoidal compounds with high yields up to 94%. We proposed the reaction mechanism, and investigated the physical properties of four fused quinoidal materials based on highly electron-rich fused aromatic compounds, which are scarce to be synthesized by the traditional method. Furthermore, these fused quinoidal materials were utilized in field-effect transistors, achieving high electron mobilities up to 1.33 cm2 V-1 s-1. We provide an effective synthetic approach to expand the library of high-performance n-type small-molecule semiconductors.