Self-terminating, heterogeneous solid-electrolyte interphase enables reversible Li-ether cointercalation in graphite anodes.

Ether solvents are suitable for formulating solid-electrolyte interphase (SEI)-less ion-solvent cointercalation electrolytes in graphite for Na-ion and K-ion batteries. However, ether-based electrolytes have been historically perceived to cause exfoliation of graphite and cell failure in Li-ion batteries. In this study, we develop strategies to achieve reversible Li-solvent cointercalation in graphite through combining appropriate Li salts and ether solvents. Specifically, we design 1M LiBF4 1,2-dimethoxyethane (G1), which enables natural graphite to deliver ~91% initial Coulombic efficiency and >88% capacity retention after 400 cycles. We captured the spatial distribution of LiF at various length scales and quantified its heterogeneity. The electrolyte shows self-terminated reactivity on graphite edge planes and results in a grainy, fluorinated pseudo-SEI. The molecular origin of the pseudo-SEI is elucidated by ab initio molecular dynamics (AIMD) simulations. The operando synchrotron analyses further demonstrate the reversible and monotonous phase transformation of cointercalated graphite. Our findings demonstrate the feasibility of Li cointercalation chemistry in graphite for extreme-condition batteries. The work also paves the foundation for understanding and modulating the interphase generated by ether electrolytes in a broad range of electrodes and batteries.

Reducing postoperative hypothermia in infants: Quality improvement in China.

BACKGROUND: Unintended postoperative hypothermia in infants is associated with increased mortality and morbidity. We noted consistent hypothermia postoperatively in more than 60% of our neonatal intensive care (NICU) babies. Therefore, we set out to determine whether a targeted quality improvement (QI) project could decrease postoperative hypothermia rates in infants. OBJECTIVES: Our SMART aim was to reduce postoperative hypothermia (<36.5°C) in infants from 60% to 40% within 6 months. METHODS: This project was approved by IRB at Guangzhou Women and Children's Medical Center, China. The QI team included multidisciplinary healthcare providers in China and QI experts from Children's Hospital of Philadelphia, USA. The plan-do-study-act (PDSA) cycles included establishing a perioperative-thermoregulation protocol, optimizing the transfer process, and staff education. The primary outcome and balancing measures were, respectively, postoperative hypothermia and hyperthermia (axillary temperature < 36.5°C, >37.5°C). Data collected was analyzed using control charts. The factors associated with a reduction in hypothermia were explored using regression analysis. RESULTS: There were 295 infants in the project. The percentage of postoperative hypothermia decreased from 60% to 37% over 26 weeks, a special cause variation below the mean on the statistical process control chart. Reduction in hypothermia was associated with an odds of 0.17 (95% CI: 0.06-0.46; p <.001) for compliance with the transport incubator and 0.24 (95% CI: 0.1-0.58; p =.002) for prewarming the OR ambient temperature to 26°C. Two infants had hyperthermia. CONCLUSIONS: Our QI project reduced postoperative hypothermia without incurring hyperthermia through multidisciplinary team collaboration with the guidance of QI experts from the USA.

Comprehensive Atlas of Alternative Splicing Reveals NSRP1 Promoting Adipogenesis through CCDC18.

Alternative splicing (AS) plays a crucial role in regulating gene expression, function, and diversity. However, limited reports exist on the identification and comparison of AS in Eastern and Western pigs. Here, we analyzed 243 transcriptome data from eight tissues, integrating information on transcription factors (TFs), selection signals, splicing factors (SFs), and quantitative trait loci (QTL) to comprehensively study alternative splicing events (ASEs) in pigs. Five ASE types were identified, with Mutually Exclusive Exon (MXE) and Skipped Exon (SE) ASEs being the most prevalent. A significant portion of genes with ASEs (ASGs) showed conservation across all eight tissues (63.21-76.13% per tissue). Differentially alternative splicing genes (DASGs) and differentially expressed genes (DEGs) exhibited tissue specificity, with blood and adipose tissues having more DASGs. Functional enrichment analysis revealed coDASG_DEGs in adipose were enriched in pathways associated with adipose deposition and immune inflammation, while coDASG_DEGs in blood were enriched in pathways related to immune inflammation and metabolism. Adipose deposition in Eastern pigs might be linked to the down-regulation of immune-inflammation-related pathways and reduced insulin resistance. The TFs, selection signals, and SFs appeared to regulate ASEs. Notably, ARID4A (TF), NSRP1 (SF), ANKRD12, IFT74, KIAA2026, CCDC18, NEXN, PPIG, and ROCK1 genes in adipose tissue showed potential regulatory effects on adipose-deposition traits. NSRP1 could promote adipogenesis by regulating alternative splicing and expression of CCDC18. Conducting an in-depth investigation into AS, this study has successfully identified key marker genes essential for pig genetic breeding and the enhancement of meat quality, which will play important roles in promoting the diversity of pork quality and meeting market demand.

Reversible Switch in Charge Storage Enabled by Selective Ion Transport in Solid Electrolyte Interphase.

Solid-electrolyte interphases (SEIs) in advanced rechargeable batteries ensure reversible electrode reactions at extreme potentials beyond the thermodynamic stability limits of electrolytes by insulating electrons while allowing the transport of working ions. Such selective ion transport occurs naturally in biological cell membranes as a ubiquitous prerequisite of many life processes and a foundation of biodiversity. In addition, cell membranes can selectively open and close the ion channels in response to external stimuli (e.g., electrical, chemical, mechanical, and thermal), giving rise to "gating" mechanisms that help manage intracellular reactions. We wondered whether the chemistry and structure of SEIs can mimic those of cell membranes, such that ion gating can be replicated. That is, can SEIs realize a reversible switching between two electrochemical behaviors, i.e., the ion intercalation chemistry of batteries and the ion adsorption of capacitors? Herein, we report such SEIs that result in thermally activated selective ion transport. The function of open/close gate switches is governed by the chemical and structural dynamics of SEIs under different thermal conditions, with precise behaviors as conducting and insulating interphases that enable battery and capacitive processes within a finite temperature window. Such an ion gating function is synergistically contributed by Arrhenius-activated ion transport and SEI dissolution/regrowth. Following the understanding of this new mechanism, we then develop an electrochemical method to heal the SEI layer in situ. The knowledge acquired in this work reveals the possibility of hitherto unknown biomimetic properties of SEIs, which will guide us to leverage such complexities to design better SEIs for future battery chemistries.

Prognostic value of circulating tumor cells associated with white blood cells in solid cancer: a systematic review and meta-analysis of 1471 patients with solid tumors.

BACKGROUND: The clinical relevance of circulating tumor cell-white blood cell (CTC-WBC) clusters in cancer prognosis is a subject of ongoing debate. This study aims to unravel their contentious predictive value for patient outcomes. METHODS: We conducted a comprehensive literature search of PubMed, Embase, and Cochrane Library up to December 2022. Eligible studies that reported survival outcomes and examined the presence of CTC-WBC clusters in solid tumor patients were included. Hazard ratios (HR) were pooled to assess the association between CTC-WBC clusters and overall survival (OS), as well as progression-free survival (PFS)/disease-free survival (DFS)/metastasis-free survival (MFS)/recurrence-free survival (RFS). Subgroup analyses were performed based on sampling time, treatment method, detection method, detection system, and cancer type. RESULTS: A total of 1471 patients from 10 studies were included in this meta-analysis. The presence of CTC-WBCs was assessed as a prognostic factor for overall survival and PFS/DFS/MFS/RFS. The pooled analysis demonstrated that the presence of CTC-WBC clusters was significantly associated with worse OS (HR = 2.44, 95% CI: 1.74-3.40, P < 0.001) and PFS/DFS/MFS/RFS (HR = 1.83, 95% CI: 1.49-2.24, P < 0.001). Subgroup analyses based on sampling time, treatment method, detection method, detection system, cancer type, and study type consistently supported these findings. Further analyses indicated that CTC-WBC clusters were associated with larger tumor size (OR = 2.65, 95% CI: 1.58-4.44, P < 0.001) and higher alpha-fetoprotein levels (OR = 2.52, 95% CI: 1.50-4.22, P < 0.001) in hepatocellular carcinoma. However, no significant association was found between CTC-WBC clusters and TNM stage, depth of tumor invasion, or lymph node metastasis in the overall analysis. CONCLUSIONS: CTC-WBC clusters are negative predictors for OS and PFS/DFS/MFS/RFS in patients with solid tumors. Monitoring CTC-WBC levels may provide valuable information for predicting disease progression and guiding treatment decisions.

[The evolution of approach in the resuscitation of neonates born with meconium-stained amniotic fluid: a tale of two countries, China and U.S.A., in the past 60 years]. / 羊水胎粪污染新生儿复苏的前世今生：过去60年中美两国的演变史.

Neonates born through meconium-stained amniotic fluid (MSAF) may develop complications including meconium aspiration syndrome, persistent pulmonary hypertension of newborn and death. The approach to the resuscitation of these neonates has significantly evolved for the past few decades. Initially, under direct visualization technique, neonates with MSAF were commonly suctioned below the vocal cords soon after delivery. Since 2015, Neonatal Resuscitation Program (NRP®) of the American Academy of Pediatrics has recommended against "routine" endotracheal suctioning of non-vigorous neonates with MSAF but favored immediate resuscitation with positive pressure ventilation via face-mask bagging. However, the China neonatal resuscitation 2021 guidelines continue to recommend routine endotracheal suctioning of non-vigorous neonates born with MSAF at birth. This review article discusses the differences and the rationales in the approach in the resuscitation of neonates with MSAF between Chinese and American NRP® guidelines over the past 60 years.

Circular RNA MTCL1 promotes advanced laryngeal squamous cell carcinoma progression by inhibiting C1QBP ubiquitin degradation and mediating beta-catenin activation.

BACKGROUND: Circular RNAs (circRNAs) are involved in regulatory processes of ubiquitination and deubiquitination in various tumors at post-transcriptional epigenetic modification level. However, the underlying mechanism and its biological functions of circRNAs in the advanced laryngeal squamous cell carcinoma (LSCC) remain obscure. METHODS: RNA sequencing and quantitative real-time PCR (qRT-PCR) assays were applied to screen for circRNAs differentially expressed in LSCC tissues and cell lines. The candidate RNA-binding proteins and target signalling pathway were detected by RNA pull-down and mass spectrometry, in situ hybridization (ISH), immunohistochemistry (IHC), qRT-PCR assays, and bioinformatics analysis. The functional roles of these molecules were investigated using in vitro and in vivo experiments including EdU, transwell, wound healing, western blot assays, and the xenograft mice models. The molecular mechanisms were identified using RNA pull-down assays, RNA immunoprecipitation (RIP), Co-IP, ISH, Ubiquitination assay, bioinformatics analysis, and the rescue experiments. RESULTS: Here, we unveil that microtubule cross-linking factor 1 circRNA (circMTCL1, circ0000825) exerts its critical oncogenic functions by promoting complement C1q-binding protein (C1QBP)-dependent ubiquitin degradation and subsequently activating Wnt/ß-catenin signalling in laryngeal carcinoma initiation and development. Specifically, circMTCL1 was remarkably up-regulated in the paired tissues of patients with LSCC (n = 67), which predicted a worse clinical outcome. Functionally, circMTCL1 exerted oncogenic biological charactersistics by promoting cell proliferative capability and invasive and migrative abilities. Ectopic circMTCL1 augumented cell proliferation, migration, and invasion of LSCC cells, and this effect could be reversed by C1QBP knocking down in vitro and in vivo. Mechanistically, circMTCL1 directly recruited C1QBP protein by harboring the specific recognized sequence (+ 159 - + 210), thereby accelerating the translation of C1QBP expression by inhibiting its ubiquitin-proteasome-mediated degradation. Importantly, the direct interaction of C1QBP with ß-catenin protein was enhanced via suppressing the ß-catenin phosphorylation and accelerating its accumulation in cytoplasm and nucleus. CONCLUSION: Our findings manifested a novel circMTCL1-C1QBP-ß-catenin signaling axis involving in LSCC tumorigenesis and progression, which shed new light on circRNAs-ubiquitous acidic glycoprotein mediated ubiquitin degradation and provided strategies and targets in the therapeutic intervention of LSCC.

Engineering Hierarchical Architecture of Metal-Organic Frameworks for Highly Efficient Overall CO2 Photoreduction.

Previous studies on syntheses of metal-organic frameworks (MOFs) for photocatalytic CO2 reduction are mainly focused on the exquisite control over the net topology and the functionality of metal clusters/organic building blocks. This contribution demonstrates that the rational design of MOF-based photocatalyst can be further extended to the hierarchical structure at micrometer scales well beyond the conventional MOF design at the molecular level. By taking advantage of the disparity of two selective MOFs in nucleation kinetics, a hierarchical core-shell MOF@MOF structure is successfully constructed through a simple one-pot synthesis. Besides inheriting the high porosity, crystallinity, and robustness of parent MOFs, the obtained heterojunction exhibits extended photoresponse, optimized band alignment with large overpotential, and greatly enhanced photogenerated charge separation, which would be hardly realized by the merely molecular-level assembly. As a result, the challenging overall CO2 photoreduction is achieved, which generates a record high HCOOH production (146.0 µmol/g/h) without using any sacrificial reagents. Moreover, the core-shell structure exhibits a more effective use of photogenerated electrons than the individual MOFs. This work shows that harnessing the hierarchical architecture of MOFs present a new and effective alternative to tuning the photocatalytic performance at a mesoscopic level.

Variable focus convex microlens array on K9 glass substrate based on femtosecond laser processing and hot embossing lithography.

We propose a high-precision method for the fabrication of variable focus convex microlens arrays on K9 glass substrate by combining femtosecond laser direct writing and hot embossing lithography. A sapphire master mold with a blind cylindrical hole array was prepared first by femtosecond laser ablation. The profile control of microlenses dependent on the temperature and the diameter of the blind hole in the sapphire mold was investigated. The curvature radius of the microlens decreased with temperature and increased with diameter. Uniform convex microlens arrays were fabricated with good imaging performance. Further, variable focus convex microlens arrays were fabricated by changing the diameter of the blind hole in sapphire, which produced the image at variable z planes. This method provides a highly precise fabrication of convex microlens arrays and is well suited for batch production of micro-optical elements.

CTNNB1-related neurodevelopmental disorder in a Chinese population: A case series.

CTNNB1-related disorder is an autosomal dominant neurodevelopmental disorder characterized by a variable degree of cognitive impairment, microcephaly, truncal hypotonia, peripheral spasticity, visual defects, and dysmorphic features. In this case series, we report the clinical and molecular findings of nine Chinese patients affected by CTNNB1-related disorders. The facial features of these affected individuals appear to resemble what had been previously described, with thin upper lip (77.8%) and hypoplastic alae nasi (77.8%) being the most common. Frequently reported clinical characteristics in our cohort include developmental delay (100%), peripheral spasticity (88.9%), truncal hypotonia (66.7%), microcephaly (66.7%), and dystonia (44.4%). While various eye manifestations were reported, two affected individuals (22.2%) in our cohort had familial exudative vitreoretinopathy. One of the affected individuals had craniosynostosis, a feature not reported in the literature before. To our knowledge, this is the first reported Chinese case series of CTNNB1-related neurodevelopmental disorders. Further studies are required to look into whether ethnic differences play a role in phenotypic variations.

Droplet Tweezers Based on the Hydrophilic-Hydrophobic Interface Structure and Their Biological Application.

Droplet controllable operation has wide applications in microfluidics, biomedicine, microreactors, and other fields. Droplets can spontaneously transfer from a high-energy state to a low-energy state, but how to reverse transfer the droplets is a difficult task. In this article, we use a special hydrophilic-hydrophobic interphase structure (HHIS) to achieve this reverse transfer. We specifically study the critical conditions under which droplet transfer can be achieved. The length of the hydrophilic surface in this structure and the hydrophilic/hydrophobic properties of the surface must be in the appropriate range. Based on this, an optimized structure used to transfer droplets was designed. Finally, we carried out research on biological applications and successfully achieved the transfer of droplets from zebrafish eggs and zebrafish larvae. This unique method is low-cost, biofriendly, and highly applicable to various surfaces, illustrating the great potential in chemical and biological analysis.

Resveratrol Triggered the Quick Self-Assembly of Gallic Acid into Therapeutic Hydrogels for Healing of Bacterially Infected Wounds.

Programing self-assembly of naturally bioactive molecules has been a wide topic of great significance for biomedical uses. Despite the fact that plant-derived polyphenols with catechol or pyrogallol moieties have been widely studied to construct nanocomplexes or nanocoatings via self-polymerization, there is no report on the self-assembly of these polyphenols into therapeutic hydrogels for potential applications. Here, we reported that adding a very small amount of resveratrol (Res) into the gallic acid (GA) aqueous solution could trigger the quick self-assembly of GA to form a fibrous hydrogel within 5 min through hydrogen bonds and π-π interactions. The length of GA/Res (GR) fibrils in gels varied from 100 to 1000 microns, with a diameter of around 1 µm. Notably, these GR hydrogels showed excellent colloid stability, providing better slow release and outstanding biocompatibility. Also, in vivo experiments indicated the hydrogels had high antibacterial effects and excellent wound healing capabilities in a total skin defect model via regulating the expression of inflammatory factors (IL-6, IL-1ß, and TNF-α) due to the release of therapeutic agents (GA and Res) into the matrix. Overall, our results provide a new strategy to accelerate self-assembly of GA by adding Res to form hydrogels, which is further proved as a promising therapeutic carrier for wound healing.

Efficient Separation and Recovery of Petroleum Hydrocarbon from Oily Sludge by a Combination of Adsorption and Demulsification.

The treatment of oily sludge (OS) can not only effectively solve environmental pollution but also contribute to the efficient use of energy. In this study, the separation effect of OS was analyzed through sodium lignosulfonate (SL)-assisted sodium persulfate (S/D) treatment. The effects of SL concentration, pH, temperature, solid-liquid ratio, revolving speed, and time on SL adsorption solubilization were analyzed. The effects of sodium persulfate dosage, demulsification temperature, and demulsification time on sodium persulfate oxidative demulsification were analyzed. The oil removal efficiency was as high as 91.28%. The results showed that the sediment was uniformly and finely distributed in the S/D-treated OS. The contact angle of the sediment surface was 40°, and the initial apparent viscosity of the OS was 56 Pa·s. First, the saturated hydrocarbons and aromatic hydrocarbons on the sediment surface were adsorbed by the monolayer adsorption on SL. Stubborn, cohesive oil agglomerates were dissociated. Sulfate radical anion (SO4-·) with a high oxidation potential, was formed from sodium persulfate. The oxidation reaction occurred between SO4-· and polycyclic aromatic hydrocarbons. A good three-phase separation effect was attained. The oil recovery reached 89.65%. This provides theoretical support for the efficient clean separation of oily sludge.

[Investigation and analysis of imported medicinal materials at Chinese border ports].

Imported medicinal materials are an important part of Chinese medicinal resources. To be specific, about 10% of the around 600 commonly used Chinese medicinal materials are from abroad, and the introduction of foreign medicinal materials has promoted the development of Chinese medicine. Amid the advancement of reform and opening up and the "Belt and Road" Initiative, major headway has been made in the cross-border trade in China, bringing opportunities for the import of medicinal materials from border ports. However, for a long time, there is a lack of systematic investigation on the types of exotic medicinal materials at border ports. In the fourth national census of traditional Chinese medicine resources, National Resource Center for Chinese Materia Medica, China Academy of Chinese Medical Sciences, together with several organizations, investigated the nearly 40 border ports, Chinese medicinal material markets, and border trade markets in 6 provinces/autonomous regions in China for the first time and recorded the types, sources, circulation, and the transaction characteristics of imported medicinal materials. Moreover, they invited experts to identify the origins of the collected 237 medicinal materials. In addition, the status quo and the problems of the medicinal materials were summarized. This study is expected to lay a basis for clarifying the market and origins of imported medicinal materials as well as the scientific research on and supervision of them.

Partial Metalation of Porphyrin Moieties in Hydrogen-Bonded Organic Frameworks Provides Enhanced CO2 Photoreduction Activity.

In natural photosynthesis, the architecture of multiproteins integrates more chromophores than redox centers and simultaneously creates a well-controlled environment around the active site. Herein, we demonstrate that these features can be emulated in a prototype hydrogen-bonded organic framework (HOF) through simply varying the proportion of metalated porphyrin in the structure. Further studies demonstrate that changing the metalloporphyrin content not only realizes a fine tuning of the photosensitizer/catalyst ratio, but also alters the microenvironment surrounding the active site and the charge separation efficiency. As a result, the obtained material achieves the challenging overall CO2 reduction with a high HCOOH production rate (29.8 µmol g-1 h-1 , scavenger free), standing out from existing competitors. This work unveils that the degree of metalation is vital to the catalytic activity of the porphryinic framework, presenting as a new strategy to optimize the performance of heterogeneous catalysts.

Spatially Directed Biosynthesis of Quantum Dots via Spidroin Templating in Escherichia coli.

Spatially directed synthesis of quantum dots (QDs) is intriguing yet challenging in organisms, due to the dispersed feature of templating biomolecules and precursors. Whether this task could be accomplished by biomolecular condensates, an emerging type of membraneless compartments in cells remains unknown. Here we report synthetic protein condensates for templated synthesis of QDs in bacterium Escherichia coli. This was realized by overexpression of spider silk protein to bind precursor ions and recruit other necessary components, which induced the spidroin to form more ß-sheet structures for assembly and maturation of the protein condensates. This in turn enabled formation and co-localization of the fluorescent QDs to "light up" the condensates, and alleviated cytotoxicity of the precursor heavy metal ions and resulting QDs. Thus, our results suggest a new strategy for nanostructure synthesis and deposition in subcellular compartments with great potential for in situ applications.

Exosomes-mediated transfer of long noncoding RNA LINC01133 represses bladder cancer progression via regulating the Wnt signaling pathway.

Bladder cancer (BC), as one of the most common malignant cancers of the urinary system, has a high incidence and mortality rates. Recently, increasing studies have indicated that exosomes can mediate cellular communication in assorted cancers, including BC. Long noncoding RNAs (lncRNAs) have also been confirmed to take part in the regulation of many cancers. Long intergenic non-protein coding RNA 1133 (LINC01133) is an lncRNA and its roles in several cancers have been revealed. However, the functions of exosomes and LINC01133 in BC are still not elucidated. In our research, functional assays were conducted to evaluate the function of LINC01133, as well as the influence of exosomes and LINC01133 on BC cells. Western blot assay, immunofluorescence assay, electron microscope, and nanoparticle tracking analysis were applied for detecting the characteristics of exosomes. Bioinformatics tools and quantitative reverse-transcription polymerase chain reaction were performed to test the expression of LINC01133 in BC cells and exosomes of the immortalized human uroepithelial cell line (SV-HUC-1). Luciferase reporter assay was performed to measure the activity of the Wnt pathway. We discovered that LINC01133 expression was high in exosomes of SV-HUC-1 and low in that of BC cells. Additionally, exosomes restrained cell viability, proliferation, migration, and invasion. Similarly, LINC01133 exerted the same function on BC cells. In addition, the Wnt signaling pathway could be inactivated by LINC01133. Finally, in vivo experiments demonstrated that cell growth could be suppressed by overexpressed LINC01133. In short, exosomes-mediated transfer of lncRNA LINC01133 repressed BC progression via regulating the Wnt signaling pathway.

Molecular Dynamics Study of Binary Nanodroplet Evaporation on a Heated Homogeneous Substrate.

The evaporation mechanism of miscible binary nanodroplets from heated homogeneous surfaces was studied by molecular dynamics simulations, which has never been studied before. The binary droplets contain a hydrophilic component (type-2 particles) and a hydrophobic component (type-3 particles). It is shown that liquid-liquid interaction strength (ε23) and hydrophilic particle number fraction (φ) have great influence on the surface tension, wetting characteristics, evaporation patterns, evaporation rate, and local mass flux. It is observed that when ε23 ≥ 1, or φ ≈ 0.5, the evaporation mode is the constant-contact-angle mode. Otherwise, it is the mixed mode. We found that the evaporation rate becomes faster when φ and ε23 increase. The droplets become more hydrophilic when φ increases, which promotes heat transfer efficiency between the liquid-solid interface. Besides, a larger ε23 promotes the heat transfer inside the droplet. The mass transfer to the vapor phase occurs preferentially in the vicinity of TPCL (three phase contact line) in the hydrophilic systems (θ < θc), where θc is the critical contact angle, while in most hydrophobic systems (θ > θc), the mass flux close to the TPCL is suppressed. We found that θc ∈ (102°-106°), which is different from the theoretical one, θc = 90°. The discrepancy is attributed to the existence of the adsorption layer near the TPCL.

Investigation of Capillary Filling Dynamics of Multicomponent Fluids in Straight and Periodically Constricted Microchannels.

An extensive study of capillary flow of fluids with various viscosities in straight and periodically constricted microchannels with different surface wettability is presented. Capillary filling speed in hydrophilic, less hydrophilic, and hydrophobic microchannels were experimentally monitored and compared with the Washburn theoretical model. For all liquids, a linear relationship was found between the square of propagation distance and time, which is expected for Newtonian fluids. Experimental results indicated slower velocity compared to the theoretical prediction due to simplifications of the Washburn model. Capillary filling speed of fluids into long-fluororinated chain silane modified channels confirmed the expected lyophobic nature of the coating (i.e., not favorable for either hydrophilic or hydrophobic liquids). Presence of the precursor film ahead of the three-phase contact line in the microscopic level was demonstrated. White light and fluorescent images confirmed the presence of precursor film and capillary evaporation at the interface. Evaporation enhanced the deviation between experimental and theoretical results due to continuous wettability alteration of penetrating fluid.

Structural characterization and discrimination of Paris polyphylla var. yunnanensis by a molecular networking strategy coupled with ultra-high-performance liquid chromatography with quadrupole time-of-flight mass spectrometry.

RATIONALE: Paris polyphylla var. yunnanensis (Franch) Hand Mazz (PPY) is a traditional Chinese medicine with antitumor, antibacterial, hemostatic, and anthelmintic activities. Identification of the chemical composition in PPY is helpful to discover its active ingredients and can be used to establish its quality control protocols. METHODS: The composition of PPY was identified using ultra-high-performance liquid chromatography combined with quadrupole time-of-flight mass spectrometry (UHPLC/QTOF-MS/MS) coupled with a molecular networking strategy. First, the UHPLC/QTOF-MS/MS approach was optimized for chemical compound profiling. Then, the MS data were processed using PeakView™ combined with an in-house database to quickly characterize the secondary metabolites. Finally, molecular networking excavated new molecular weights to discover unknown or trace natural products based on the characteristics of each cluster. RESULTS: A total of 222 compounds, including 77 isospirostanols, 2 spirostanols, 19 furostanols, 10 pseudospirostanols, 6 cholesterols, 10 C21 steroids, 5 insect metamorphosis hormones, 3 plant sterols, 6 five-ring triterpenoids, 4 flavonoids, 8 fatty acids, 2 phenylpropanoids, and 8 other compounds, were characterized in PPY by comparing their main fragmentation characteristics and pathways with the literature data, and 62 of them, 54 steroidals and 8 phenylpropanoids, were discovered or tentatively identified for the first time. CONCLUSIONS: This study extended the application of a molecular networking strategy to traditional herbal medicines and developed a molecular networking based screening approach with a significant increase in efficiency for the discovery and identification of trace novel natural products.