Rational Design of a Hydrophilic Core-Hydrophobic Shell Yarn-Based Solar Evaporator with an Underwater Aerophilic Surface for Self-Floating and High-Performance Dynamic Water Purification.

Interfacial solar vapor generation holds great promise for alleviating the global freshwater crisis, but its real-world application is limited by the efficiently choppy water evaporation and industrial production capability. Herein, a self-floating solar evaporator with an underwater aerophilic surface is innovatively fabricated by weaving core-shell yarns via mature weaving techniques. The core-shell yarns possess capillary water channels in the hydrophilic cotton core and can trap air in the hydrophobic electrospinning nanofiber shell when submerged underwater, simultaneously realizing controllable water supplies, stable self-flotation, and great thermal insulation. Consequently, the self-floating solar evaporator achieves an evaporation rate of 2.26 kg m-2 h-1 under 1 sun irradiation, with a reduced heat conduction of 70.18 W m-2. Additionally, for the first time, a solar evaporator can operate continuously in water with varying waveforms and intensities over 24 h, exhibiting an outdoor cumulative evaporation rate of 14.17 kg m-2 day-1.

Mobility Selective Ion Soft-Landing and Characterization Enabled Using Structures for Lossless Ion Manipulation.

While conventional ion-soft landing uses the mass-to-charge (m/z) ratio to achieve molecular selection for deposition, here we demonstrate the use of Structures for Lossless Ion Manipulation (SLIM) for mobility-based ion selection and deposition. The dynamic rerouting capabilities of SLIM were leveraged to enable the rerouting of a selected range of mobilities to a different SLIM path (rather than MS) that terminated at a deposition surface. A selected mobility range from a phosphazene ion mixture was rerouted and deposited with a current pulse (∼150 pA) resembling its mobility peak. In addition, from a mixture of tetra-alkyl ammonium (TAA) ions containing chain lengths of C5-C8, selected chains (C6, C7) were collected on a surface, reconstituted into solution-phase, and subsequently analyzed with a SLIM-qToF to obtain an IMS/MS spectrum, confirming the identity of the selected species. Further, this method was used to characterize triply charged tungsten-polyoxometalate anions, PW12O403- (WPOM). The arrival time distribution of the IMS/MS showed multiple peaks associated with the triply charged anion (PW12O403-), of which a selected ATD was deposited and imaged using TEM. Additionally, the identity of the deposited WPOM was ascertained using energy-dispersive (EDS) spectroscopy. Further, we present theory and computations that reveal ion landing energies, the ability to modulate the energies, and deposition spot sizes.

Making Nanofiber Membrane Stand on End to Construct Vertically Interfacial Evaporators for Efficient Solar Evaporation, Omnidirectional Solar Absorption, and Ultrahigh-Salinity Brine Desalination.

Solar-driven interfacial desalination is widely considered to be a promising technology to address the global water crisis. This study proposes a novel electrospun nanofiber-based all-in-one vertically interfacial solar evaporator endowed with a high steam generation rate, steady omnidirectional evaporation, and enduring ultrahigh-salinity brine desalination. In particular, the electrospun nanofiber is collected into the tubular structure, followed by spraying with a dense crosslinked poly(vinyl alcohol) film, which renders them sufficiently strong for the preparation of a vertically array evaporator. The integrated evaporator made an individual capillary as a unit to form multiple thermal localization interfaces and steam dissipation channels, realizing zone heating of water. Thus a high steam generation rate exceeding 4.0 kg m-2 h-1 in pure water is demonstrated even under omnidirectional sunlight, and outperforms existing evaporators. Moreover, salt ions in the photothermal layer can be effectively transported to the water in capillaries and subsequently exchanged with the bulk water due to the strong action of capillary force, which ensures an ultrahigh desalination rate (≈12.5 kg m-2 h-1 under 3 sun) in 25 wt% concentration brine over 300 min. As such, this work provides a meaningful roadmap for the development of state-of-the-art solar-driven interfacial desalination.

Isolation and identification of NEAU-CP5: A seed-endophytic strain of B. velezensis that controls tomato bacterial wilt.

Bacterial wilt of tomato caused by Ralstonia solanacearum is a critical soilborne disease that drastically reduces yield. In the current study, an endophytic strain NEAU-CP5 with strong antagonistic activity against R. solanacearum was isolated from tomato seeds and characterized. The strain was identified as Bacillus velezensis based on 16S rRNA gene and whole genome sequence analysis. NEAU-CP5 can secrete amylase, protease, and cellulase, and also produce known antibacterial metabolites, including cyclo (leucylprolyl), cyclo (phenylalanyl-prolyl), cyclo (Pro-Gly), 3-benzyl-2,5-piperazinedione, pentadecanoic acid, eicosane, 2-methyoic acid, isovaleric acid, dibuty phthalate, and esters of fatty acids (HFDU), which may be responsible for its strong antibacterial activity. Fourteen gene clusters associated with antibacterial properties were also identified in the whole genome sequence of NEAU-CP5. Pot experiment demonstrated that the application of 108 CFU/mL NEAU-CP5 on tomato plants significantly reduced the incidence of tomato bacterial wilt by 68.36 ± 1.67 %. NEAU-CP5 also increased the activity of defense-related enzymes (CAT, POD, PPO, SOD, and PAL) in tomato plants. This is the first report of an effective control of bacterial wilt on tomato plants by B. velezensis and highlights the potential of NEAU-CP5 as a potential biocontrol agent for the management of tomato bacterial wilt.

CCDC88C, an O-GalNAc glycosylation substrate of GALNT6, drives breast cancer metastasis by promoting c-JUN-mediated CEMIP transcription.

Coiled-coil domain containing 88C (CCDC88C) is a component of non-canonical Wnt signaling, and its dysregulation causes colorectal cancer metastasis. Dysregulated expression of CCDC88C was observed in lymph node metastatic tumor tissues of breast cancer. However, the role of CCDC88C in breast cancer metastasis remains unclear. To address this, the stable BT549 and SKBR3 cell lines with CCDC88C overexpression or knockdown were developed. Loss/gain-of-function experiments suggested that CCDC88C drove breast cancer cell motility in vitro and lung and liver metastasis in vivo. We found that CCDC88C led to c-JUN-induced transcription activation. Overlapping genes were identified from the genes modulated by CCDC88C and c-JUN. CEMIP, one of these overlapping genes, has been confirmed to confer breast cancer metastasis. We found that CCDC88C regulated CEMIP mRNA levels via c-JUN and it exerted pro-metastatic capabilities in a CEMIP-dependent manner. Moreover, we identified the CCDC88C as a substrate of polypeptide N-acetylgalactosaminyltransferase 6 (GALNT6). GALNT6 was positively correlated with CCDC88C protein abundance in the normal breast and breast cancer tissues, indicating that GALNT6 might be associated with expression patterns of CCDC88C in breast cancer. Our data demonstrated that GALNT6 maintained CCDC88C stability by promoting its O-linked glycosylation, and the modification was critical for the pro-metastatic potential of CCDC88C. CCDC88C also could mediate the pro-metastatic potential of GALNT6 in breast cancer. Collectively, our findings uncover that CCDC88C may increase the risk of breast cancer metastasis and elucidate the underlying molecular mechanisms.

Isoptericola luteus sp. nov., a novel yellow bacterium isolated from soil.

An aerobic, non-motile, Gram-stain-positive bacterium, designated strain NEAU-Y5T, was isolated from a soil sample collected from Northeast Agricultural University, Heilongjiang province. Phylogenetic analysis based on 16S rRNA gene sequences indicated that strain NEAU-Y5T belonged to the genus and showed high 16S rRNA sequence similarity to Isoptericola variabilis (98.9 %), Isoptericola nanjingensis (98.9 %), Isoptericola cucumis (98.5 %), Isoptericola hypogeus (98.5 %), Isoptericola dokdonensis (98.5 %), Isoptericola jiangsuensis (98.3 %), and Isoptericola halalbus (98.1 %), followed by other members of the genus Isoptericola (<98 %), and phylogenetically clustered with I. dokdonensis and I. jiangsuensis. Strain NEAU-Y5T was found to grow at 4-40 °C (optimum, 28 °C), pH 6.0-12.0 (optimum, pH 7.0), and tolerated 0-6 % NaCl (w/v). The cell-wall peptidoglycan type was l-Lys-d-Asp. The whole-cell hydrolysates contained glucose, galactose, and ribose. The major polar lipids were diphosphatidylglycerol, phosphatidylethanolamine, hydroxyphosphatidylethanolamine, phosphatidylinositol, phosphatidylinositol mannoside, and glucosamine unknown phospholipid. Major fatty acids were anteiso-C15 : 0 and anteiso-C17 : 0. The predominant menaquinone was MK-9(H4). The DNA G+C content was 73.4 mol%. The digital DNA-DNA hybridization and average nucleotide identity values between strain NEAU-Y5T and the type strains of the genus Isoptericola ranged from 18.6 to 23.5 % and from 77.3 to 81.6 %, respectively. Based on morphological, physiological, chemotaxonomic, and phylogenetic data, as well as digital DNA-DNA hybridization and average nucleotide identity values, the novel strain NEAU-Y5T could be differentiated from its closest relatives. Therefore, the strain represents a novel species of the genus Isoptericola, for which the name Isoptericola luteus sp. nov. is proposed. The type strain is NEAU-Y5T (=CCTCC AA 2019087T=DSM 110637T).

α-Ketoglutarate alleviates osteoarthritis by inhibiting ferroptosis via the ETV4/SLC7A11/GPX4 signaling pathway.

Osteoarthritis (OA) is the most common degenerative joint disorder that causes disability in aged individuals, caused by functional and structural alterations of the knee joint. To investigate whether metabolic drivers might be harnessed to promote cartilage repair, a liquid chromatography-mass spectrometry (LC-MS) untargeted metabolomics approach was carried out to screen serum biomarkers in osteoarthritic rats. Based on the correlation analyses, α-ketoglutarate (α-KG) has been demonstrated to have antioxidant and anti-inflammatory properties in various diseases. These properties make α-KG a prime candidate for further investigation of OA. Experimental results indicate that α-KG significantly inhibited H2O2-induced cartilage cell matrix degradation and apoptosis, reduced levels of reactive oxygen species (ROS) and malondialdehyde (MDA), increased superoxide dismutase (SOD) and glutathione (GSH)/glutathione disulfide (GSSG) levels, and upregulated the expression of ETV4, SLC7A11 and GPX4. Further mechanistic studies observed that α-KG, like Ferrostatin-1 (Fer-1), effectively alleviated Erastin-induced apoptosis and ECM degradation. α-KG and Fer-1 upregulated ETV4, SLC7A11, and GPX4 at the mRNA and protein levels, decreased ferrous ion (Fe2+) accumulation, and preserved mitochondrial membrane potential (MMP) in ATDC5 cells. In vivo, α-KG treatment inhibited ferroptosis in OA rats by activating the ETV4/SLC7A11/GPX4 pathway. Thus, these findings indicate that α-KG inhibits ferroptosis via the ETV4/SLC7A11/GPX4 signaling pathway, thereby alleviating OA. These observations suggest that α-KG exhibits potential therapeutic properties for the treatment and prevention of OA, thereby having potential clinical applications in the future.

Cisternostomy is not beneficial to reduce the occurrence of post-traumatic hydrocephalus in Traumatic Brain Injury.

BACKGROUND: The Cisternostomy is a novel surgical concept in the treatment of Traumatic Brain Injury (TBI), which can effectively drain the bloody cerebrospinal fluid from the skull base cistern, reduce the intracranial pressure, and improve the return of bone flap, but its preventive role in post-traumatic hydrocephalus (PTH) is unknow. The purpose of this paper is to investigate whether Cisternostomy prevents the occurrence of PTH in patients with moderate and severe TBI. METHODS: A retrospective analysis of clinical data of 86 patients with moderate and severe TBI from May 2019 to October 2021 was carried out in the Brain Trauma Center of Tianjin Huanhu Hospital. Univariate analysis was performed to examine the gender, age, preoperative Glasgow Coma Scale (GCS) score, preoperative Rotterdam CT score, decompressive craniectomy rate, intracranial infection rate, the incidence of subdural fluid, and incidence of hydrocephalus in patients between the Cisternostomy group and the non-Cisternostomy surgery group. we also analyzed the clinical outcome indicators like GCS at discharge,6 month GOS-E and GOS-E ≥ 5 in two groups.Additionaly, the preoperative GCS score, decompressive craniectomy rate, age, and gender of patients with PTH and non hydrocephalus were compared. Further multifactorial logistic binary regression was performed to explore the risk factors for PTH. Finally, we conducted ROC curve analysis on the statistically significant results from the univariate regression analysis to predict the ability of each risk factor to cause PTH. RESULTS: The Cisternostomy group had a lower bone flap removal rate(48.39% and 72.73%, p = 0.024)., higer GCS at discharge(11.13 ± 2.42 and 8.93 ± 3.31,p = 0.000) and better 6 month GOS-E(4.55 ± 1.26 and 3.95 ± 1.18, p = 0.029)than the non-Cisternostomy group However, there was no statistical difference in the incidence of hydrocephalus between the two groups (25.81% and 30.91%, p = 0.617). Moreover, between the hydrocephalus group and no hydrocephalus group,there were no significant differences in the incidence of gender, age, intracranial infection, and subdural fluid. While there were statistical differences in peroperative GCS score, Rotterdam CT score, decompressive craniectomy rate, intracranial infection rate, and the incidence of subdural fluid in the two groups, there was no statistical difference in the percentage of cerebral cisterns open drainage between the hydrocephalus group and no hydrocephalus group (32.00% and 37.70%, p = 0.617). Multifactorial logistic binary regression analysis results revealed that the independent risk factors for PTH were intracranial infection (OR = 18.460, 95% CI: 1.864-182.847 p = 0.013) and subdural effusion (OR = 10.557, 95% CI: 2.425-35.275 p = 0.001). Further, The ROC curve analysis showed that peroperative GCS score, Rotterdam CT score and subdural effusion had good ACU(0.785,0.730,and 0.749), with high sensitivity and specificity to predict the occurrence of PTH. CONCLUSIONS: Cisternostomy may decrease morbidities associated with removal of the bone flap and improve the clinical outcome, despite it cannot reduce the disability rate in TBI patients.Intracranial infection and subdural fluid were found to be the independent risk factors for PTH in patients with TBI,and the peroperative GCS score, Rotterdam CT score and subdural effusion had higher sensitivity and specificity to predict the occurrence of PTH. And more importantly, no correlation was observed between open drainage of the cerebral cisterns and the occurrence of PTH, indicating that Cisternostomy may not be beneficial in preventing the occurrence of PTH in patients with moderate and severe TBI.

PLAC8 contributes to the malignant behaviors of cervical cancer cells by activating the SOX4-mediated AKT pathway.

Cervical cancer (CC) is the primary cancer-related cause of morbidity and mortality in women. Previous studies have shown that placenta-specific 8 (PLAC8) has different functions in multiple malignancies. This study aimed to explore the function and regulatory mechanism of PLAC8 in CC. Bioinformatics and immunohistochemical analyses demonstrated that PLAC8 was significantly upregulated in CC tissues compared with normal tissues. Gain/loss-of-function experiments showed that siRNA-mediated knockdown of PLAC8 suppressed cell migration and invasion, while PLAC8 overexpression promoted cell motility. Moreover, PLAC8 was revealed to affect the epithelial-mesenchymal transition (EMT) process by upregulating epithelial (E)-cadherin and decreasing the expression of mesenchymal markers of EMT, including vimentin, zinc finger E-box binding homeobox 1 (ZEB1), neural (N)-cadherin, matrix metalloproteinase-9 (MMP-9), and MMP-2 in PLAC8-silenced cells. PLAC8 activated the AKT pathway, as proven by the downregulation of p-AKTSer473 and p-AKTThr308 expression after PLAC8 knockdown. Furthermore, PLAC8 overexpression upregulated the expression of sex-determining region Y-related high-mobility group box transcription factor 4 (SOX4), which is reported to mediate the activation of the AKT pathway, and SOX4 deficiency reversed the cellular functions caused by PLAC8 overexpression. Overall, the present study indicates that PLAC8 may facilitate CC development by activating the SOX4-mediated AKT pathway, suggesting that PLAC8 may serve as a potential biomarker for CC treatment.

Gradient-Charged Hydrogels for Highly Efficient Solar Steam Generation and Desalination.

Solar-driven interface desalination (SDID) is a promising and sustainable technology that produces freshwater from brine. Ionic hydrogels are effective evaporators, providing enhanced interaction with water and ions due to the charged groups on hydrophilic polymer networks. In this study, we developed a hydrogel-based solar steam generator with a gradient-charged (GC) structure for desalination. The gradient-charged groups' distribution on the hydrogels creates gradients of free water and osmotic pressure, realizing rapid water supplement as well as desalination of concentrated brine. Consequently, the GC hydrogel demonstrated an exceptional water evaporation rate, achieving a value as high as 2.61 kg m-2 h-1 in pure water and 1.72 kg m-2 h-1 on treating with 20 wt % NaCl solution under one sun illumination. Following the substantial solar-driven evaporation, impurities, including salt and other pollutants, were removed, thereby ensuring the purity of the condensed water. Overall, the GC hydrogel-based evaporator is a promising solution for SDID to achieve effective and sustainable water desalination.

The cohesive properties and pyrolysis mechanism of an aprotic ionic liquid tetrabutylammonium bis(trifluoromethanesulfonyl)imide.

As the cohesive properties (such as the enthalpy of sublimation) of solid organic salts (or ionic liquids, ILs) are unmeasurable, a method of their indirect determination is proposed in this paper. For this purpose, the thermogravimetric analysis (TGA) and differential scanning calorimetric analysis (DSC) were carried out over a wide range of temperatures. In this study, the mathematical relationship of the thermodynamic properties between the liquid and solid phases of ILs is established using the Born-Fajans-Haber cycle, in which the sum of the vaporization enthalpy of ILs, melting enthalpy and the enthalpy of solid-solid phase transition is regarded as the sublimation enthalpy of solid organic salts. With this method, the cohesive properties of tetrabutylammonium bis(trifluoromethanesulfonyl)imide ([N4444][NTf2]), which is an aprotic IL, were successfully obtained. Additionally, the difference between the lattice energy and the cohesive energy was employed to quantitatively calculate the charge separation distance of single ion pair (r12) in the gas phase of ionic liquids for the first time, which can serve as a standard methodology to measure the closeness in distance between the anion and the cation in a gas phase ion pair. The pyrolysis mechanism of [N4444][NTf2] was also explored.

Polar Nitrated Aromatic Compounds in Urban Fine Particulate Matter: A Focus on Formation via an Aqueous-Phase Radical Mechanism.

Polar nitrated aromatic compounds (pNACs) are key ambient brown carbon chromophores; however, their formation mechanisms, especially in the aqueous phase, remain unclear. We developed an advanced technique for pNACs and measured 1764 compounds in atmospheric fine particulate matter sampled in urban Beijing, China. Molecular formulas were derived for 433 compounds, of which 17 were confirmed using reference standards. Potential novel species with up to four aromatic rings and a maximum of five functional groups were found. Higher concentrations were detected in the heating season, with a median of 82.6 ng m-3 for Σ17pNACs. Non-negative matrix factorization analysis indicated that primary emissions particularly coal combustion were dominant in the heating season. While in the non-heating season, aqueous-phase nitration could generate abundant pNACs with the carboxyl group, which was confirmed by their significant association with the aerosol liquid water content. Aqueous-phase formation of 3- and 5-nitrosalicylic acids instead of their isomer of 4-hydroxy-3-nitrobenzoic acid suggests the existence of an intermediate where the intramolecular hydrogen bond favors kinetics-controlled NO2• nitration. This study provides not only a promising technique for the pNAC measurement but also evidence for their atmospheric aqueous-phase formation, facilitating further evaluation of pNACs' climatic effects.

Multi-Scale Nanoarchitectured Fibrous Networks for High-Performance, Self-Sterilization, and Recyclable Face Masks.

Airborne particulate matter (PM) pollutants, especially with nanoscale size, have caused serious public health issues. The global demand for high-performance and recyclable face masks is increasing dramatically, especially during the COVID-19 pandemic. However, present masks suffer from low-efficiency interception of PM0.3 /pathogen, limited air permeability, and incapacity to reuse and recycle. Here, multi-scale nanoarchitectured nanofiber/carbon nanotube (NF/CNT) networks are constructed by a needleless-electrospinning/spraying-netting strategy, enabling well-dispersed CNT networks (diameter ≈ 25 nm) welded on charged nanofibrous scaffolds (diameter > 100 nm) layer by layer. The optimized NF/CNT networks possess a fluffy structure with narrow-distribution small pores (size ≈ 400 nm), "free molecular flow" behavior, and electrostatic adsorption property, thereby exhibiting high filtration efficiency (>99.994% PM0.3 removal) and low resistance (<0.05% atmosphere pressure). Furthermore, they demonstrate reliable and ultra-fast photothermal-driven self-sterilization (>99.986% in 5 min) under 1 sun and electrothermal-driven self-sterilization (>99.9999% in 2 min) in sunless scenes owing to their unique nanoarchitecture. Most importantly, the abandoned NF/CNT filters can be fully recycled as high-performance solar vapor generators to desalinate seawater (3.56 L m-2 d-1 ). This work offers a fascinating solution to reduce disease transmission, resource consumption, and environmental burdens.

AutoCCS: automated collision cross-section calculation software for ion mobility spectrometry-mass spectrometry.

MOTIVATION: Ion mobility spectrometry (IMS) separations are increasingly used in conjunction with mass spectrometry (MS) for separation and characterization of ionized molecular species. Information obtained from IMS measurements includes the ion's collision cross section (CCS), which reflects its size and structure and constitutes a descriptor for distinguishing similar species in mixtures that cannot be separated using conventional approaches. Incorporating CCS into MS-based workflows can improve the specificity and confidence of molecular identification. At present, there is no automated, open-source pipeline for determining CCS of analyte ions in both targeted and untargeted fashion, and intensive user-assisted processing with vendor software and manual evaluation is often required. RESULTS: We present AutoCCS, an open-source software to rapidly determine CCS values from IMS-MS measurements. We conducted various IMS experiments in different formats to demonstrate the flexibility of AutoCCS for automated CCS calculation: (i) stepped-field methods for drift tube-based IMS (DTIMS), (ii) single-field methods for DTIMS (supporting two calibration methods: a standard and a new enhanced method) and (iii) linear calibration for Bruker timsTOF and non-linear calibration methods for traveling wave based-IMS in Waters Synapt and Structures for Lossless Ion Manipulations. We demonstrated that AutoCCS offers an accurate and reproducible determination of CCS for both standard and unknown analyte ions in various IMS-MS platforms, IMS-field methods, ionization modes and collision gases, without requiring manual processing. AVAILABILITY AND IMPLEMENTATION: https://github.com/PNNL-Comp-Mass-Spec/AutoCCS. SUPPLEMENTARY INFORMATION: Supplementary data are available at Bioinformatics online. Demo datasets are publicly available at MassIVE (Dataset ID: MSV000085979).

A Separation-Sensing Platform Performing Accurate Diagnosis of Jaundice in Complex Biological Tear Fluids.

The detection of biomarkers in tears has aroused great interest owing to the advantages of non-invasive and rapid collection. The combination of ultrasensitivity and label-free detection of surface-enhanced Raman spectroscopy (SERS) sensors is expected to achieve real-time diagnosis in home medical care. However, the surface of SERS sensors is susceptible to biofouling and inactivation by biological impurities in tears, resulting in rapid degradation of sensitivity, limiting the commercialization of point-of-care devices. Herein, a binary nanosphere array with dual properties is constructed as a separation-sensing platform for the diagnosis of target molecules in tears. The upper part of the structure is composed of Au nanoparticles (AuNPs) and a sputtering Au layer, which can bind the target molecules that interact with Au and provide high-strength and high-density SERS hotspots. The lower half is an inactive SiO2 nanosphere array with periodic large pores that allows biological impurities to penetrate the lower part and be separated from the target analyte. Furthermore, this substrate was integrated into homemade tear kits, enabling simultaneous tear collection, pre-separation, and detection. Combined with the Raman spectra of tears and LDA analysis, we successfully identified patients with jaundice in clinics. This platform is expected to provide an opportunity for early disease screening based on biological fluids.

New insights into the fine-scale history of western-eastern admixture of the northwestern Chinese population in the Hexi Corridor via genome-wide genetic legacy.

Trans-Eurasian cultural and genetic exchanges have significantly influenced the demographic dynamics of Eurasian populations. The Hexi Corridor, located along the southeastern edge of the Eurasian steppe, served as an important passage of the ancient Silk Road in Northwest China and intensified the transcontinental exchange and interaction between populations on the Central Plain and in Western Eurasia. Historical and archeological records indicate that the Western Eurasian cultural elements were largely brought into North China via this geographical corridor, but there is debate on the extent to which the spread of barley/wheat agriculture into North China and subsequent Bronze Age cultural and technological mixture/shifts were achieved by the movement of people or dissemination of ideas. Here, we presented higher-resolution genome-wide autosomal and uniparental Y/mtDNA SNP or STR data for 599 northwestern Han Chinese individuals and conducted 2 different comprehensive genetic studies among Neolithic-to-present-day Eurasians. Genetic studies based on lower-resolution STR markers via PCA, STRUCTURE, and phylogenetic trees showed that northwestern Han Chinese individuals had increased genetic homogeneity relative to northern Mongolic/Turkic/Tungusic speakers and Tibeto-Burman groups. The genomic signature constructed based on modern/ancient DNA further illustrated that the primary ancestry of the northwestern Han was derived from northern millet farmer ancestors, which was consistent with the hypothesis of Han origin in North China and more recent northwestward population expansion. This was subsequently confirmed via excess shared derived alleles in f3/f4 statistical analyses and by more northern East Asian-related ancestry in the qpAdm/qpGraph models. Interestingly, we identified one western Eurasian admixture signature that was present in northwestern Han but absent from southern Han, with an admixture time dated to approximately 1000 CE (Tang and Song dynasties). Generally, we provided supporting evidence that historic Trans-Eurasian communication was primarily maintained through population movement, not simply cultural diffusion. The observed population dynamics in northwestern Han Chinese not only support the North China origin hypothesis but also reflect the multiple sources of the genetic diversity observed in this population.

Double-Layer Nitrogen-Rich Two-Dimensional Anionic Uranyl-Organic Framework for Cation Dye Capture and Catalytic Fixation of Carbon Dioxide.

A novel two-dimensional double-layer anionic uranyl-organic framework, U-TBPCA {[NH2(CH3)2][(UO2)(TBPCA)], where H3TBPCA = 4,4',4″-s-triazine-1,3,5-triyltripamino-methylene-cyclohexane-carboxylate}, with abundant active sites and stability was obtained by assembling UO2(NO3)2·6H2O and a triazine tricarboxylate linker, TBPCA3-. Due to the flexibility of the ligand and diverse coordination modes between carboxyl groups and uranyl ions, U-TBPCA exhibits an intriguing topological structure and steric configuration. This double-layer anionic uranyl-organic framework is highly porous and can be used for selective adsorption of cationic dyes. Due to the presence of high-density metal ions and basic -NH- groups, U-TBPCA acts as an effective heterogeneous catalyst for the cycloaddition reaction of carbon dioxide with epoxy compounds. Moreover, the various modes of coordination between the tricarboxylic ligand and uranyl ion were studied by density functional theory calculations, and several simplified models were established to probe the influence of hydrogen bonding between carbon dioxide and U-TBPCA on the ability of U-TBPCA to bind carbon dioxide. This work should aid in improving our understanding of the coordination behavior of uranyl ion as well as the development and utilization of new actinide materials.

Assessing Collision Cross Section Calibration Strategies for Traveling Wave-Based Ion Mobility Separations in Structures for Lossless Ion Manipulations.

The collision cross section (CCS) is an important property that aids in the structural characterization of molecules. Here, we investigated the CCS calibration accuracy with traveling wave ion mobility spectrometry (TWIMS) separations in structures for lossless ion manipulations (SLIM) using three sets of calibrants. A series of singly negatively charged phospholipids and bile acids were calibrated in nitrogen buffer gas using two different TW waveform profiles (square and sine) and amplitudes (20, 25, and 30 V0-p). The calibration errors for the three calibrant sets (Agilent tuning mixture, polyalanine, and one assembled in-house) showed negligible differences using a sine-shaped TW waveform. Calibration errors were all within 1-2% of the drift tube ion mobility spectrometry (DTIMS) measurements, with lower errors for sine waveforms, presumably due to the lower average and maximum fields experienced by ions. Finally, ultrahigh-resolution multipass (long path length) SLIM TWIMS separations demonstrated improved CCS calibration for phospholipid and bile acid isomers.

Ion Mobility Spectrometry with High Ion Utilization Efficiency Using Traveling Wave-Based Structures for Lossless Ion Manipulations.

Ion packets introduced from gates, ion funnel traps, and other conventional ion injection mechanisms produce ion pulse widths typically around a few microseconds or less for ion mobility spectrometry (IMS)-based separations on the order of 100 milliseconds. When such ion injection techniques are coupled with ultralong path length traveling wave (TW)-based IMS separations (i.e., on the order of seconds) using structures for lossless ion manipulations (SLIMs), typically very low ion utilization efficiency is achieved for continuous ion sources [e.g., electrospray ionization (ESI)]. Even with the ability to trap and accumulate much larger populations of ions than being conventionally feasible over longer time periods in SLIM devices, the subsequent long separations lead to overall low ion utilization. Here, we report the use of a highly flexible SLIM arrangement, enabling concurrent ion accumulation and separation and achieving near-complete ion utilization with ESI. We characterize the ion accumulation process in SLIM, demonstrate >98% ion utilization, and show both increased signal intensities and measurement throughput. This approach is envisioned to have broad utility to applications, for example, involving the fast detection of trace chemical species.

Ultra-High-Resolution Ion Mobility Separations Over Extended Path Lengths and Mobility Ranges Achieved using a Multilevel Structures for Lossless Ion Manipulations Module.

Over the past few years, structures for lossless ion manipulations (SLIM) have used traveling waves (TWs) to move ions over long serpentine paths that can be further lengthened by routing the ions through multiple passages of the same path. Such SLIM "multipass" separations provide unprecedentedly high ion mobility resolving powers but are ultimately limited in their ion mobility range because of the range of mobilities spanned in a single pass; that is, higher mobility ions ultimately "overtake" and "lap" lower mobility ions that have experienced fewer passes, convoluting their arrival time distribution at the detector. To achieve ultrahigh resolution separations over broader mobility ranges, we have developed a new multilevel SLIM possessing multiple stacked serpentine paths. Ions are transferred between SLIM levels through apertures (or ion escalators) in the SLIM surfaces. The initial multilevel SLIM module incorporates four levels and three interlevel ion escalator passages, providing a total path length of 43.2 m. Using the full path length and helium buffer gas, high resolution separations were achieved for Agilent tuning mixture phosphazene ions over a broad mobility range (K0 ≈ 3.0 to 1.2 cm2/(V*s)). High sensitivity was achieved using "in-SLIM" ion accumulation over an extended trapping region of the first SLIM level. High transmission efficiency of ions over a broad mobility range (e.g., K0 ≈ 3.0 to 1.67 cm2/(V*s)) was achieved, with transmission efficiency rolling off for the lower mobility ions (e.g., K0 ≈ 1.2 cm2/(V*s)). Resolving powers of up to ∼560 were achieved using all four ion levels to separate reverse peptides (SDGRG1+ and GRGDS1+). A complex mixture of phosphopeptides showed similar coverage could be achieved using one or all four SLIM levels, and doubly charged phosphosite isomers not significantly separated using one SLIM level were well resolved when four levels were used. The new multilevel SLIM technology thus enables wider mobility range ultrahigh-resolution ion mobility separations and expands on the ability of SLIM to obtain improved separations of complex mixtures with high sensitivity.