ABSTRACT
A series of 1,2,4-triazolo-quinazolinones and 1,2-benzisothiazolone derivatives (S1-S12) were successfully synthesized as environmentally friendly alternatives to copper-based antifouling paints using N-alkylation, cyclocondensation, and one-pot three-component and amide coupling reactions. The monoclinic structure of single-crystal 1,2,4-triazolo-quinazolin-acetic acid (S8) was confirmed by single-crystal X-ray diffraction analysis. All the synthesized molecules were studied for their in silico molecular docking interactions with three target proteins, namely, RbmA, ToxR, and Bap. Following that, the antialgal activity was assessed against two types of marine algae: Chlorella sp. and Chaetoceros curvisetus. The minimal inhibitory concentration and zone of inhibition have been used to evaluate the antibacterial activities of S1-S12 against both marine Gram-positive (Staphylococcus aureus) and Gram-negative (Vibrio parahemolyticus and Vibrio vulnificus) bacteria. Additionally, antifouling studies have been done on all the compounds, and among them, 1,2,4-triazolo-quinazolinyl-acetate (S7), 1,2,4-triazolo-quinazolinyl-acetic acid (S8), 1,2,4-triazolo-quinazolinyl-oxobutanoate (S9), benzo[d]isothiazolyl butanoate (S10), benzo[d]isothiazolyl-acetic acid (S11), and 1,2,4-triazolo-quinazolinyl-acetyl-benzo[d]isothiazolone (S12) exhibited good antialgal, antibacterial, and antifouling activities.
ABSTRACT
Double-crystal monochromators (DCMs) are one of the most critical optical devices in beamlines at synchrotron sources, directly affecting the quality of the beam energy and position. As the performance of synchrotron light sources continues to improve, higher demands are placed on the stability of DCMs. This paper proposes a novel adaptive vibration control method combining variational modal decomposition (VMD) and filter-x normalized least mean squares (FxNLMS), ensuring DCM stability under random engineering disturbance. Firstly, the sample entropy of the vibration signal is selected as the fitness function, and the number of modal components k and the penalty factor α are optimized by a genetic algorithm. Subsequently, the vibration signal is decomposed into band frequencies that do not overlap with each other. Eventually, each band signal is individually governed by the FxNLMS controller. Numerical results have demonstrated that the proposed adaptive vibration control method has high convergence accuracy and excellent vibration suppression performance. Furthermore, the effectiveness of the vibration control method has been verified with actual measured vibration signals of the DCM.
ABSTRACT
Sea surface roughness (SSR) is a key physical parameter in studies of air-sea interactions and the ocean dynamics process. The SSR quantitative inversion model based on multi-angle sun glitter (SG) images has been proposed recently, which will significantly promote SSR observations through multi-angle remote-sensing platforms. However, due to the sensitivity of the sensor view angle (SVA) to SG, it is necessary to determine the optimal imaging angle and their combinations. In this study, considering the design optimization of imaging geometry for multi-angle remote-sensing platforms, we have developed an error transfer simulation model based on the multi-angle SG remote-sensing radiation transmission and SSR estimation models. We simulate SSR estimation errors at different imaging geometry combinations to evaluate the optimal observation geometry combination. The results show that increased SSR inversion accuracy can be obtained with SVA combinations of 0° and 20° for nadir- and backward-looking SVA compared with current combinations of 0° and 27.6°. We found that SSR inversion prediction error using the proposed model and actual SSR inversion error from field buoy data are correlated. These results can provide support for the design optimization of imaging geometry for multi-angle ocean remote-sensing platforms.
ABSTRACT
The electrochemical conversion of carbon dioxide (CO2) to valuable chemicals is gaining significant attention as a pragmatic solution for achieving carbon neutrality and storing renewable energy in a usable form. Recent research increasingly focuses on designing electrocatalysts that specifically convert CO2 into ethanol, a desirable product due to its high-energy density, ease of storage, and portability. However, achieving high-efficiency ethanol production remains a challenge compared to ethylene (a competing product with a similar electron configuration). Existing electrocatalytic systems often suffer from limitations such as low energy efficiency, poor stability, and inadequate selectivity toward ethanol. Inspired by recent progress in the field, this review explores fundamental principles and material advancements in CO2 electroreduction, emphasizing strategies for ethanol production over ethylene. We discuss electrocatalyst design, reaction mechanisms, challenges, and future research directions. These advancements aim to bridge the gap between current research and industrialized applications of this technology.
ABSTRACT
In response to societal developments and the growing demand for high-energy-density battery systems, alkali metal batteries (AMBs) have emerged as promising candidates for next-generation energy storage. Despite their high theoretical specific capacity and output voltage, AMBs face critical challenges related to high reactivity with electrolytes and unstable interphases. This review, from the perspective of electrolytes, analyzes AMB failure mechanisms, including interfacial side reactions, active materials loss, and metal dendrite growth. It then reviews recent advances in innovative electrolyte molecular designs, such as ether, ester, sulfone, sulfonamide, phosphate, and salt, aimed at overcoming the above-mentioned challenges. Finally, we propose the current molecular design principles and future promising directions that can help future precise electrolyte molecular design.
ABSTRACT
Uncontrollable zinc (Zn) plating and hydrogen evolution greatly undermine Zn anode reversibility. Previous electrolyte designs focus on suppressing H2O reactivity, however, the accumulation of alkaline byproducts during battery calendar aging and cycling still deteriorates the battery performance. Here, we present a direct strategy to tackle such problems using a strong Brønsted acid, bis(trifluoromethanesulfonyl)imide (HTFSI), as the electrolyte additive. This approach reformulates battery interfacial chemistry on both electrodes, suppresses continuous corrosion reactions and promotes uniform Zn deposition. The enrichment of hydrophobic TFSI- anions at the Zn|electrolyte interface creates an H2O-deficient micro-environment, thus inhibiting Zn corrosion reactions and inducing a ZnS-rich interphase. This highly acidic electrolyte demonstrates high Zn plating/stripping Coulombic efficiency up to 99.7% at 1 mA cm-2 ( > 99.8% under higher current density and areal capacity). Additionally, Zn | |ZnV6O9 full cells exhibit a high capacity retention of 76.8% after 2000 cycles.
ABSTRACT
Constraining the electrochemical reactivity of free solvent molecules is pivotal for developing high-voltage lithium metal batteries, especially for ether solvents with high Li metal compatibility but low oxidation stability ( <4.0 V vs Li+/Li). The typical high concentration electrolyte approach relies on nearly saturated Li+ coordination to ether molecules, which is confronted with severe side reactions under high voltages ( >4.4 V) and extensive exothermic reactions between Li metal and reactive anions. Herein, we propose a molecular anchoring approach to restrict the interfacial reactivity of free ether solvents in diluted electrolytes. The hydrogen-bonding interactions from the anchoring solvent effectively suppress excessive ether side reactions and enhances the stability of nickel rich cathodes at 4.7 V, despite the extremely low Li+/ether molar ratio (1:9) and the absence of typical anion-derived interphase. Furthermore, the exothermic processes under thermal abuse conditions are mitigated due to the reduced reactivity of anions, which effectively postpones the battery thermal runaway.
ABSTRACT
Although somatic cells can be reprogrammed to pluripotent stem cells (PSCs) with pure chemicals, authentic pluripotency of chemically induced pluripotent stem cells (CiPSCs) has never been achieved through tetraploid complementation assay. Spontaneous reprogramming of spermatogonial stem cells (SSCs) was another non-transgenic way to obtain PSCs, but this process lacks mechanistic explanation. Here, we reconstructed the trajectory of mouse SSC reprogramming and developed a five-chemical combination, boosting the reprogramming efficiency by nearly 80- to 100-folds. More importantly, chemical induced germline-derived PSCs (5C-gPSCs), but not gPSCs and chemical induced pluripotent stem cells, had authentic pluripotency, as determined by tetraploid complementation. Mechanistically, SSCs traversed through an inverted pathway of in vivo germ cell development, exhibiting the expression signatures and DNA methylation dynamics from spermatogonia to primordial germ cells and further to epiblasts. Besides, SSC-specific imprinting control regions switched from biallelic methylated states to monoallelic methylated states by imprinting demethylation and then re-methylation on one of the two alleles in 5C-gPSCs, which was apparently distinct with the imprinting reprogramming in vivo as DNA methylation simultaneously occurred on both alleles. Our work sheds light on the unique regulatory network underpinning SSC reprogramming, providing insights to understand generic mechanisms for cell-fate decision and epigenetic-related disorders in regenerative medicine.
Subject(s)
Induced Pluripotent Stem Cells , Pluripotent Stem Cells , Male , Mice , Animals , Cellular Reprogramming/genetics , Tetraploidy , Pluripotent Stem Cells/metabolism , Induced Pluripotent Stem Cells/metabolism , DNA Methylation , Spermatogonia/metabolism , Germ Cells/metabolismABSTRACT
The properties of mRNA lipid nanoparticles (mRNA-LNPs), including size, empty particles, morphology, storage stability, and transfection potency, are critically dependent on the preparation methods. Here, a Two-step tangential-flow filtration (TFF) method was successfully employed to improve the properties of mRNA-LNPs during the preparation process. This method involves an additional ethanol removal step prior to the particle fusion process. Notably, this innovative approach has yielded mRNA-LNPs with larger particles, a reduced proportion of empty LNPs, optimized storage stability (at least 6 months at 2-8 °C), improved in vitro transfection efficiency, and minimized distribution in the heart and blood in vivo. In summary, this study represents the implementation of the innovative Two-step TFF method in the preparation of mRNA-LNPs. Our findings indicate substantial enhancements in the properties of our mRNA-LNPs, specifically with regard to the percentage of empty LNPs, stability, transfection efficiency, and in vivo distribution. These improvements have the potential to optimize their industrial applicability and expand their clinical use.
Subject(s)
Lipids , Nanoparticles , RNA, Messenger/genetics , Liposomes , RNA, Small Interfering/geneticsABSTRACT
Background: Autophagy has been implicated as a crucial component in spermatogenesis, and autophagy dysfunction can lead to reproductive disorders in animal models, including yeast, C. elegans and mice. However, the sophisticated transcriptional networks of autophagic genes throughout human spermatogenesis and their biological significance remain largely uncharacterized. Methods: We profiled the transcriptional signatures of autophagy-related genes during human spermatogenesis by assessing specimens from nine fertile controls (including two normal persons and seven obstructive azoospermia (OA) patients) and one nonobstructive azoospermia (NOA) patient using single-cell RNA sequencing (scRNA-seq) analysis. Dysregulation of autophagy was confirmed in two additional NOA patients by immunofluorescence staining. Gene knockdown was used to identify the role of Cst3 in autophagy during spermatogenesis. Results: Our data uncovered a unique, global stage-specific enrichment of autophagy-related genes. Human-mouse comparison analysis revealed that the stage-specific expression pattern of autophagy-related genes was highly conserved in mammals. More importantly, dysregulation of some clusters of autophagy-related genes was observed in NOA patients, suggesting the association of autophagy with male infertility. Cst3, a human-mouse conserved and autophagy-related gene that is actively expressed in spermatogonia and early spermatocytes, was found to regulate spermatogonial stem cell (SSC) maintenance and subsequent male germ cell development. Knockdown of Cst3 increased autophagic activity in mouse SSCs and subsequently suppressed the transcription of SSC core factors such as Oct4, Id1, and Nanos3, which could be efficiently rescued by manipulating autophagic activity. Conclusions: Our study provides comprehensive insights into the global transcriptional signatures of autophagy-related genes and confirms the importance of autophagy homeostasis in SSC maintenance and normal spermatogenesis, opening new avenues for further dissecting the significance of the autophagy regulatory network in spermatogenesis as well as male infertility.
Subject(s)
Autophagy/genetics , Azoospermia/genetics , Cystatin C/genetics , Spermatogenesis/genetics , Adult , Adult Germline Stem Cells/metabolism , Gene Expression Profiling , Gene Knockdown Techniques , Gene Regulatory Networks , Humans , Male , Meiosis/genetics , Middle Aged , RNA-Seq , Single-Cell Analysis , Vas DeferensABSTRACT
Mammalian male germ cell development is a stepwise cell-fate transition process; however, the full-term developmental profile of male germ cells remains undefined. Here, by interrogating the high-precision transcriptome atlas of 11,598 cells covering 28 critical time-points, we demonstrate that cell-fate transition from mitotic to post-mitotic primordial germ cells is accompanied by transcriptome-scale reconfiguration and a transitional cell state. Notch signaling pathway is essential for initiating mitotic arrest and the maintenance of male germ cells' identities. Ablation of HELQ induces developmental arrest and abnormal transcriptome reprogramming of male germ cells, indicating the importance of cell cycle regulation for proper cell-fate transition. Finally, systematic human-mouse comparison reveals potential regulators whose deficiency contributed to human male infertility via mitotic arrest regulation. Collectively, our study provides an accurate and comprehensive transcriptome atlas of the male germline cycle and allows for an in-depth understanding of the cell-fate transition and determination underlying male germ cell development.