Nanostructured Gold/Bismutite Hybrid Heterocatalysts for Plasmon-Enhanced Photosynthesis of Ammonia

Nitrogen (N₂) reduction to produce ammonia (NH₃) is one of the most important chemical processes globally. Nowadays, the Haber–Bosch process is the main industrial procedure for artificial N₂ fixation, which requires extremely harsh synthetic conditions and large energy consumption resulting in massive emission of greenhouse gas. Hence, an alternative photosynthesis of NH₃ under mild condition, which is sustainable and less energy consuming, would be highly desirable. In this study, Au nanoparticles modified (BiO)₂CO₃ nanodisks were fabricated through a facile hydrothermal method followed by chemical bath deposition and investigated for the photocatalytic reduction of N₂ in a pure water system at atmospheric pressure and room temperature. The induction of Au nanoparticles can dramatically enhance the light trapping as well as charge separation in the Au/(BiO)₂CO₃ hybrid, thereby promoting overall energy conversion efficiency. The synergetic effect of the nanostructured gold/bismutite hybrid results in high catalytic activity and exhibits high performance for artificial photosynthesis of ammonia

Communication-Efficient Nonparametric Quantile Regression via Random Features

This paper introduces a refined algorithm designed for distributed nonparametric quantile regression in a reproducing kernel Hilbert space (RKHS). Unlike existing nonparametric approaches that primarily address homogeneous data, our approach utilizes kernel-based quantile regression to effectively model heterogeneous data. Moreover, we integrate the concepts of random features (RF) and communication-efficient surrogate likelihood (CSL) to ensure accurate estimation and enhance computational efficiency in distributed settings. Specifically, we employ an embedding technique to map the original data into RF spaces, enabling us to construct an extended surrogate loss function. This function can be locally optimized using an iterative alternating direction method of multipliers (ADMM) algorithm, minimizing the need for extensive computation and communication within the distributed system. The paper thoroughly investigates the asymptotic properties of the distributed estimator and provides convergence rates of the excess risk. These properties are established under mild technical conditions and are comparable to state-of-the-art results in the literature. Additionally, we validate the effectiveness of the proposed algorithm through a comprehensive set of synthetic examples and a real data study, effectively highlighting its advantages and practical utility.</p

Concomitant Production of Erythritol and β‑Carotene by Engineered <i>Yarrowia lipolytica</i>

While the expansion of the erythritol production industry has resulted in unprecedented production of yeast cells, it also suffers from a lack of effective utilization. β-Carotene is a value-added compound that can be synthesized by engineered Yarrowia lipolytica. Here, we first evaluated the production performance of erythritol-producing yeast strains under two different morphologies and then successfully constructed a chassis with yeast-like morphology by deleting Mhy1 and Cla4 genes. Subsequently, β-carotene synthesis pathway genes, CarRA and CarB from Blakeslea trispora, were introduced to construct the β-carotene and erythritol coproducing Y. lipolytica strain ylmcc. The rate-limiting genes GGS1 and tHMG1 were overexpressed to increase the β-carotene yield by 45.32-fold compared with the strain ylmcc. However, increased β-carotene accumulation led to prolonged fermentation time; therefore, transporter engineering through overexpression of YTH1 and YTH3 genes was used to alleviate fermentation delays. Using batch fermentation in a 3 L bioreactor, this engineered Y. lipolytica strain produced erythritol with production, yield, and productivity values of 171 g/L, 0.56 g/g glucose, and 2.38 g/(L·h), respectively, with a concomitant β-carotene yield of 47.36 ± 0.06 mg/g DCW. The approach presented here improves the value of erythritol-producing cells and offers a low-cost technique to obtain hydrophobic terpenoids

DataSheet_1_Framing seascape connectivity modeling to prioritize marine conservation effort in China’s coastal sea.docx

Anthropogenic disturbances and climate change are projected to become leading drivers of biodiversity loss and ecological connectivity degradation in marine ecosystems. However, the lack of quantitative understanding for seascape connectivity modeling hinders our ability in providing large-scale marine conservation guidance. By applying well-established theories and tools in landscape connectivity study and marine-specific indicators, we proposed a framework to evaluate the resistance-based seascape connectivity among marine habitats and Marine Protected Areas (MPAs) across China’s coastal sea. The spatial vulnerability of marine habitats was further assessed to prioritize conservation effort. Our results showed that 82% of China’s coastal seas were covered with middle to high level of resistance for migratory marine species, mainly due to concentrated inshore anthropogenic disturbances such as ship traffic and ocean pollution. With the modeled migration distances of different species guilds from short-range (25 km) to long-range (100 km), the area percentage of connected corridors increased from 12.02% to 44.68% in the study area. Vulnerable areas were identified as high resistance (high exposure) and abundant threatened species (high sensitivity) but with small number of connected corridors (low adaptive capacity), primarily distributed in offshore regions of Yellow Sea and East China Sea. Collectively, inshore regions with high anthropogenic disturbances warrant regulation and mitigation in major coastal cities and ports. While the lack of interconnected networks for offshore regions prioritized efforts to enhance seascape connectivity through the establishment of MPA network. Sensitive species groups require more attention in future marine conservation, including threatened populations, climate refugees of marine species, and species with limited movement ranges. This study highlights the potential of developing seascape connectivity model based on landscape theories, and the importance of seascape connectivity study in guiding evidence-based marine conservation strategies.</p

Laminar Flame Speeds and Flame Instabilities of Pentanol Isomer–Air Mixtures at Elevated Temperatures and Pressures

Laminar flame speeds of three pentanol isomer (1-, 2-, and 3-pentanol)–air mixtures were measured at equivalence ratios of 0.6–1.8, initial pressures of 0.10–0.75 MPa, and initial temperatures of 393–473 K using the outwardly propagating spherical flame. A recently developed kinetic mechanism of 1-pentanol oxidation (Dagaut model) was used to simulate the laminar flame speeds of 1-pentanol–air mixtures under experimental conditions. A comparison between simulation and measurement shows that the simulation yields good agreement on the stoichiometric and fuel-rich side, but it gives lower values on the fuel-lean side. A kinetic modeling study was performed, and several rate constants of selected elemental reactions were modified on the basis of the sensitivity analysis. The modified model gives good prediction on the laminar flame speed under all experimental conditions. The modified model is also validated against the jet-stirred reactor (JSR) experimental data, and it exhibits good prediction for most species. 1-Pentanol gives the fastest laminar flame speed, followed by 3- and 2-pentanol. 2- and 3-pentanol have very close values considering the experimental uncertainty. With the increase of the pressure, the difference in the laminar flame speed among pentanol isomers is decreased. The flame instability of three pentanol isomers was also analyzed. 2- and 3-pentanol have similar instability behavior with a close density ratio, flame thickness, and Lewis number, while 1-pentanol shows slightly high instability behavior. In comparison to 2- and 3-pentanol, 1-pentanol has a smaller critical radius and Peclect number, and this suggests its high instability behavior

Systemic mRNA Delivery to the Lungs by Functional Polyester-based Carriers

Messenger RNA (mRNA) has recently come into focus as an emerging therapeutic class with great potential for protein replacement therapy, cancer immunotherapy, regenerative medicine, vaccines, and gene editing. However, the lack of effective and safe delivery methods impedes the broad application of mRNA-based therapeutics. We report a robust approach to develop efficient polymeric delivery carriers for mRNA. Lead polyesters were identified by in vitro screening of a 480-member combinatorially modified poly­(trimethylolpropane allyl ether-<i>co</i>-suberoyl chloride) library for the delivery of luciferase encoding mRNA (Luc mRNA) to IGROV1 cells. The formulation of mRNA polyplex nanoparticles (NPs) with Pluronic F127 decreased the surface charge. Although this improved the stability of mRNA nanoparticles, the delivery potency decreased with increased F127 content. Thus, we determined that NP stabilization with 5% F127 could balance the protective effects and delivery potency. 5% F127 formulated PE4K-A17-0.33C12 mRNA NPs enabled luciferase expression predominantly in the lungs after intravenous injection into mice. The efficient mRNA delivery specifically to lungs by degradable carriers suggests the potential for the treatment of pulmonary diseases

Entropy-Driven Self-Assembly of Single Quantum Dot Sensor for Catalytic Imaging of Telomerase in Living Cells

Telomerase is a highly valuable cancer diagnosis biomarker and a promising cancer therapy target. So far, most telomerase assays are limited by the involvement of tedious procedures, multiple enzymes, and complicated reaction schemes. Sensitive monitoring of low-abundant telomerase in living cells remains a challenge. Herein, we demonstrate an entropy-driven catalytic assembly of quantum dot (QD) sensors for accurate detection and imaging of telomerase activity in living cells. In this sensor, target telomerase specifically catalyzes extension of telomerase primer, and the extended primer subsequently acts as a catalyst to continuously initiate entropy-driven catalytic reaction, generating a large number of fluorophore- and biotin-labeled DNAs that can be self-assembled on the QD surface to induce an efficient Föster resonance energy transfer signal. The proposed sensor requires a single step for both recognition and amplification of the telomerase signal, eliminating the use of either protein enzymes or laborious procedures. Taking advantage of the inherent superiority of single-molecule fluorescence detection and high amplification efficiency of the entropy-driven reaction, this sensor demonstrates single-cell sensitivity for the in vitro assay. Moreover, it is capable of screening the telomerase inhibitor, discriminating different tumor cells from normal ones, and even real-time imaging telomerase in living cells, providing a novel platform for telomerase-associated cancer diagnosis and drug screening

Theoretical Study of Am(III) and Eu(III) Separation by a Bipyridyl Phosphate Ligand

Actinide An(III) and lanthanide Ln(III) are known to exhibit similar chemical properties; thus, it is difficult to distinguish them in the separation of highly radioactive waste liquids. One potential method to efficiently separate actinides and lanthanides involves the design and development of phosphorus–oxygen-bonded ligands with solvent extraction separation. Here, a bipyridine phosphate ligand with two isopropyl and phosphate groups is introduced to selectively extract actinides. The electronic structure, bonding properties, thermodynamic behavior, and quantum theory of atoms in molecules (QTAIM) of Am(III) and Eu(III) complexes with the bipyridine phosphate ligands were analyzed by using density functional theory (DFT) calculations. The analysis demonstrates that the Am–N bond exhibits stronger covalent characteristics than the Eu–N bond, indicating that the bipyridine phosphate ligand had better selectivity for Am(III) than for Eu(III) in terms of binding affinity. The thermodynamic analysis established the complex [ML(NO3)2(H2O)2]+ as the most stable species during the complexation process. The results indicate great potential for utilizing the bipyridine phosphate ligand for the effective separation of An(III)/Ln(III) in spent fuel reprocessing experiments

Lauric Acid/Expanded Graphite Composite Phase Change Film with High Thermal Conductivity for Thermal Management

With the rapid development of electronics toward integration and miniaturization, efficient and accurate removal of excess energy from electronics has become a major challenge. In this study, a novel expanded graphite-based composite phase change film (EL) with high thermal conductivity was synthesized to facilitate the heat dissipation of electronic devices. The expanded graphite was compressed into a thin film and then impregnated with lauric acid (LA) to form EL. The effect of pressure on the thermal performance of EL was investigated. The results show that the latent heat storage capacity of composite phase films increases with the decrease in pressure. The melting and cooling enthalpy of EL-0 reach up to 111.6 and 107.9 J/g, respectively. Meanwhile, the corresponding in-plane thermal conductivity and axial thermal conductivity reach up to 21.28 W/(m·K) and 9.70 W/(m·K), which are 54.6 and 24.9 times those of the pure LA, respectively. It is interesting that the introduction of a phase change material (PCM) improves the axial thermal conductivity in comparison with the expanded graphite film without the PCM. The obtained EL exhibits excellent leakage-proof property and long-term thermal reliability. Last, the EL utilized in the thermal management of the graphics processing unit of the laptop running decreased the temperature by 5.0 °C, implying a potential application in the thermal management of electronics

Comparison of Techniques for the Quantitation of Reductive Aroma Compounds in White Wine: Links to Sensory Analysis and Cu Fractions

Multiple analytical methodologies allow quantitation of H2S and methanethiol (MeSH) in wine, but confirmation that the determined concentrations are related to perceived off-aromas, or “reductive” faults, is yet to be provided. Fifty white wines underwent sensory evaluation and measurement of free and salt-treated H2S and MeSH concentrations by gas chromatography with sulfur chemiluminescence detection and/or gas detection tubes. The determined concentrations were compared across techniques and different analysis laboratories. Sulfhydryl off-odors in the wines were best described by boiled and rotten egg and natural gas/sewerage/durian aroma attributes. The wines with the highest ratings for both aromas had high concentrations of free H2S, free MeSH, and/or salt-treated MeSH but were unrelated to salt-treated H2S. The free sulfhydryl concentrations and their associated aromas appeared to be suppressed by specific Cu fractions in the wines. This study provides evidence of the relevant measures of reductive aroma compounds and their relation to off-odors and Cu fractions