Metagenomic analysis of individual mosquito viromes reveals the geographical patterns and drivers of viral diversity.

Mosquito transmitted viruses are responsible for an increasing burden of human disease. Despite this, little is known about the diversity and ecology of viruses within individual mosquito hosts. Here, using a meta-transcriptomic approach, we determined the viromes of 2,438 individual mosquitoes (81 species), spanning ~4,000 km along latitudes and longitudes in China. From these data we identified 393 viral species associated with mosquitoes, including 7 (putative) species of arthropod-borne viruses (that is, arboviruses). We identified potential mosquito species and geographic hotspots of viral diversity and arbovirus occurrence, and demonstrated that the composition of individual mosquito viromes was strongly associated with host phylogeny. Our data revealed a large number of viruses shared among mosquito species or genera, enhancing our understanding of the host specificity of insect-associated viruses. We also detected multiple virus species that were widespread throughout the country, perhaps reflecting long-distance mosquito dispersal. Together, these results greatly expand the known mosquito virome, linked viral diversity at the scale of individual insects to that at a country-wide scale, and offered unique insights into the biogeography and diversity of viruses in insect vectors.

A Flexible and Stretchable MXene/Waterborne Polyurethane Composite-Coated Fiber Strain Sensor for Wearable Motion and Healthcare Monitoring.

Fiber-based flexible sensors have promising application potential in human motion and healthcare monitoring, owing to their merits of being lightweight, flexible, and easy to process. Now, high-performance elastic fiber-based strain sensors with high sensitivity, a large working range, and excellent durability are in great demand. Herein, we have easily and quickly prepared a highly sensitive and durable fiber-based strain sensor by dip coating a highly stretchable polyurethane (PU) elastic fiber in an MXene/waterborne polyurethane (WPU) dispersion solution. Benefiting from the electrostatic repulsion force between the negatively charged WPU and MXene sheets in the mixed solution, very homogeneous and stable MXene/WPU dispersion was successfully obtained, and the interconnected conducting networks were correspondingly formed in a coated MXene/WPU shell layer, which makes the as-prepared strain sensor exhibit a gauge factor of over 960, a large sensing range of over 90%, and a detection limit as low as 0.5% strain. As elastic fiber and mixed solution have the same polymer constitute, and tight bonding of the MXene/WPU conductive composite on PU fibers was achieved, enabling the as-prepared strain sensor to endure over 2500 stretching-releasing cycles and thus show good durability. Full-scale human motion detection was also performed by the strain sensor, and a body posture monitoring, analysis, and correction prototype system were developed via embedding the fiber-based strain sensors into sweaters, strongly indicating great application prospects in exercise, sports, and healthcare.

In-Situ Construction of V2 O5 Nanosheet/Nitrogen-Doped Carbon Nanosheet Heterostructures with Interfacial C─O Bridging Bonds as the Cathode Material for Zn Ion Batteries.

Layered oxides are widely used as the electrode materials for metal ion batteries. However, for large radius size ions, such as Zn2+ and Al3+ , the tightly stacked layers and poor electrical conductivity of layered oxides result in restricted number of active sites and sluggish reaction kinetics. In this work, a facile in-situ construction strategy is provided to synthesize layered oxide nanosheets/nitrogen-doped carbon nanosheet (NC) heterostructure, which shows larger interlayer spacing and better electrical conductivity than the layered oxides. As a result, the Zn2+ ion diffusion inside the interlayer gallery is greatly enhanced and the storage sites inside the gallery can be better used. Meanwhile, the NC layers and oxide nanosheets are bridged by the C─O bonds to form a stable structure, which contributes to a better cycling stability than the pure layered oxides. The optimal V2 O5 @NC-400 cathode shows a capacity of 467 mA h g-1 at 0.1 A g-1 for 300 cycles, and long-term cyclic stability of 4000 cycles at 5 A g-1 with a capacity retention of 92%. All these performance parameters are among the best for vanadium oxide-based cathode materials.

Metagenomic analysis of individual mosquitos reveals the ecology of insect viruses.

Mosquito transmitted viruses are responsible for an increasing burden of human disease. Despite this, little is known about the diversity and ecology of viruses within individual mosquito hosts. Using a meta-transcriptomic approach, we analysed the virome of 2,438 individual mosquitos (79 species), spanning ~4000 km along latitudes and longitudes in China. From these data we identified 393 core viral species associated with mosquitos, including seven (putative) arbovirus species. We identified potential species and geographic hotspots of viral richness and arbovirus occurrence, and demonstrated that host phylogeny had a strong impact on the composition of individual mosquito viromes. Our data revealed a large number of viruses shared among mosquito species or genera, expanding our knowledge of host specificity of insect-associated viruses. We also detected multiple virus species that were widespread throughout the country, possibly facilitated by long-distance mosquito migrations. Together, our results greatly expand the known mosquito virome, linked the viral diversity at the scale of individual insects to that at a country-wide scale, and offered unique insights into the ecology of viruses of insect vectors.

A Gradient Lithiophilic Structure for Stable Lithium Metal Anodes with Ultrahigh Rate and Ultradeep Capacity.

Using three-dimensional current collectors (3DCC) as frameworks for lithium metal anodes (LMAs) is a promising approach to inhibit dendrite growth. However, the intrinsically accumulated current density on the top surface and limited Li-ion transfer in the interior of 3DCC still lead to the formation of lithium dendrites, which can pose safety risks. In this study, it reports that gradient lithiophilic structures can induce uniform lithium deposition within the interior of the 3DCC, greatly suppressing dendrite formation, as confirmed by COMSOL simulations and experimental results. With this concept, a gradient-structured zinc oxide-loaded copper foam (GSZO-CF) is synthesized via an easy solution-combustion method at low cost. The resulting Li@GSZO-CF symmetric cells demonstrate stable cycling performance for over 800 cycles, with an ultra-deep capacity of 10 mAh cm-2 even under an ultra-high current density of 50 mA cm-2 , the top results reported in the literature. Moreover, when combined with a LiFePO4 (LFP) cathode under a low negative/positive (N/P) capacity ratio of 2.9, the Li@GSZO-CF||LFP full cells exhibit stable performance for 200 cycles, with a discharge capacity of 130 mAh g-1 and retention of 85.5% at a charging/discharging rate of 1C. These findings suggest a promising strategy for the development of new-generation LMAs.

Total Structure, Electronic Structure and Catalytic Hydrogenation Activity of Metal-Deficient Chiral Polyhydride Cu57 Nanoclusters.

Accurate identifying and in-depth understanding of the defect sites in a working nanomaterial could hinge on establishing specific defect-activity relationships. Yet, atomically precise coinage-metal nanoclusters (NCs) possessing surface vacancy defects are scarce primarily owing to challenges in the synthesis and isolation of such defective NCs. Herein we report a mixed-ligand strategy to synthesizing an intrinsically chiral and metal-deficient copper hydride-rich NC [Cu57 H20 (PET)36 (TPP)4 ]+ (Cu57 H20 ). Its total structure (including hydrides) and electronic structure are well established by combined experimental and computational results. Crystal structure reveals Cu57 H20 features a cube-like Cu8 kernel embedded in a corner-missing metal-ligand shell of Cu49 (PET)36 (TPP)4 . Single Cu vacancy defect site occurs at one corner of the shell, evocative of mono-lacunary polyoxometalates. Theoretical calculations demonstrate that the above-mentioned point vacancy causes one surface hydride exposed as an interfacial capping µ3 -H- , which is accessible in chemical reaction, as proved by deuterated experiment. Moreover, Cu57 H20 shows catalytic activity in the hydrogenation of nitroarene. The success of this work opens the way for the research on well-defined chiral metal-deficient Cu and other metal NCs, including exploring their application in asymmetrical catalysis.

Secondary hierarchical complexity in double-stranded cluster helicates covered by NNNNN type pincer ligands.

We designed and synthesized a new tripyridine dipyrrolide pincer ligand, which could be doubly deprotonated to provide five-nitrogen-donor sites and then utilized to prepare a subnanometric chiral silver cluster. The cluster belongs to an S4 point group and shows a double-stranded helicate. DFT calculations were performed to analyze the electronic structure of the cluster. Interestingly, through hierarchical intercluster interactions, the cluster helicates evolve into complex secondary structures including a right-handed helix and a folded sheet, both of which are reminiscent of secondary structures of proteins, i.e., an α-helix and an antiparallel ß-sheet.

Multi-layer 3D Chirality and Double-Helical Assembly in a Copper Nanocluster with a Triple-Helical Cu15 Core.

Conceptually mimicking biomolecules' ability to construct multiple-helical aggregates with emergent properties and functions remains a long-standing challenge. Here we report an atom-precise 18-copper nanocluster (NC), Cu18 H(PET)14 (TPP)6 (NCS)3 (Cu18 H) which contains a pseudo D3 -symmetrical triple-helical Cu15 core. Structurally, Cu18 H may be also viewed as sandwich type of sulfur-bridged chiral copper cluster units [Cu6 -Cu6 -Cu6 ], endowing three-layered 3D chirality. More importantly, the chiral NCs are aggregated into an infinite double-stranded helix supported by intra-strand homonuclear C-H⋅⋅⋅H-C dihydrogen contacts and inter-strand C-H/π and C-H/S interactions. The unique multi-layered 3D chirality and the double-helical assembly of Cu18 H are evocative of DNA. Moreover, the collective behaviours of the aggregated NCs not only exhibit crystallization-induced emission enhancement (CIEE) and aggregation-induced emission enhancement (AIEE) effects in the deep-red region, but also efficiently catalyze electron transfer (ET) reaction. This study thus presents that hierarchical assemblies of atomically defined copper NCs could be intricate as observed for important biomolecules like DNA with emergent properties arising from aggregated behaviours.

Improved Biohythane Production from Rice Straw in an Integrated Anaerobic Bioreactor under Thermophilic Conditions.

This study evaluated the feasibility of continuous biohythane production from rice straw (RS) using an integrated anaerobic bioreactor (IABR) at thermophilic conditions. NaOH/Urea solution was employed as a pretreatment method to enhance and improve biohythane production. Results showed that the maximum specific biohythane yield was 612.5 mL/g VS, including 104.1 mL/g VS for H2 and 508.4 mL/g VS for CH4, which was 31.3% higher than the control RS operation stage. The maximum total chemical oxygen demand (COD) removal stabilized at about 86.8%. COD distribution results indicated that 2% of the total COD (in the feed) was converted into H2, 85.4% was converted to CH4, and 12.6% was retained in the effluent. Furthermore, carbon distribution analysis demonstrated that H2 production only diverted a small part of carbon, and most of the carbon flowed to the CH4 fermentation process. Upon further energy conversion analysis, the maximum value was 166.7%, 31.7 times and 12.8% higher than a single H2 and CH4 production process. This study provides a new perspective on lignocellulose-to-biofuel recovery.

Negatively Charged Holey Titania Nanosheets Added Electrolyte to Realize Dendrite-Free Lithium Metal Battery.

Electrolyte modulation and electrode structure design are two common strategies to suppress dendrites growth on Li metal anode. In this work, a self-adaptive electrode construction method to suppress Li dendrites growth is reported, which merges the merits of electrolyte modulation and electrode structure design strategies. In detail, negatively charged titania nanosheets with densely packed nanopores on them are prepared. These holey nanosheets in the electrolyte move spontaneously onto the anode under electrical field, building a mesoporous structure on the electrode surface. The as-formed porous electrode has large surface area with good lithiophilicity, which can efficiently transfer lithium ion (Li+ ) inside the electrode, and induce the genuine lithium plating/stripping. Moreover, the negative charges and nanopores on the sheets can also regulate the lithium-ion flux to promote uniform deposition of Li metal. As a result, the symmetric and full cells using the holey titania nanosheets containing electrolyte, show much better performance than the ones using electrolyte without holey nanosheets inside. This work points out a new route for the practical applications of Li-metal batteries.

A novel homozygous mutation in ACTL7A leads to male infertility.

Male infertility, a global public health problem, exhibits complex pathogenic causes and genetic factors deserve further discovery and study. We identified a novel homozygous missense mutation c.224A > C (p.D75A) in ACTL7A gene in two infertile brothers with teratozoospermia by whole-exome sequencing (WES). In vitro fertilization (IVF) and intracytoplasmic sperm injection (ICSI) showed fertilization failure of the two affected couples. The three-dimensional (3D) models showed that a small section of α-helix transformed into random coil in the mutant ACTL7A protein and mutant amino acid lacked a hydrogen bond with Ser170 amino acid. Immunofluorescence revealed that ACTL7A protein was degraded in sperms of patients. Transmission electron microscopy (TEM) analysis of sperms from the infertile patients showed that the irregular perinuclear theca (PT) and acrosomal ultrastructural defects. Furthermore, ACTL7A mutation caused abnormal localization and reduced the expression of PLCZ1 in sperms of the patients, which may be the key reasons for the fertilization failure after ICSI. Our findings expand the spectrum of ACTL7A mutations and provide novel theoretical basis for genetic counseling.

Poly(ether imide) Porous Membrane Developed by a Scalable Method for High-Performance Lithium-Sulfur Batteries: Combined Theoretical and Experimental Study.

Lithium-sulfur (Li-S) batteries are one of the emerging candidates for energy storage systems due to their high theoretical energy density and the abundance/nontoxicity/low cost of sulfur. Compared with conventional lithium-ion batteries, multiple new challenges have been brought into this advanced battery system, such as polysulfide shuttling in conventional polyolefin separators and undesired lithium dendrite formation of the Li metal anode. These issues severely affect the cell performance and impede their practical applications. Herein, we develop a poly(ether imide) (PEI)-based membrane with a sponge-like pore morphology as the separator for the Li-S battery by a simplified phase inversion method. This new separator can not only alleviate the new challenges in Li-S batteries but also exhibit excellent ion conductivity, better thermal stability, and higher mechanical strength compared to those of the conventional polypropylene (PP) separator. A combined experimental and theoretical study indicates that the sponge-like morphology of the PEI membrane and its good wettability toward the electrolyte can facilitate uniform ion transportation and suppress dendrite growth. Meanwhile, the PEI molecules exhibit a strong interaction with polysulfides and avoid their shuttling effectively. As a result, the PEI-based Li-S battery shows a much better performance from various aspects (capacity, rate capability, and cycling stability) than that of the PP-based Li-S battery, especially at high charge/discharge current densities and high sulfur loadings. Since the developed PEI membrane can be easily scaled up, this work may accelerate the practical applications of Li-S batteries from the point of separators.

Total RNA sequencing of Phlebotomus chinensis sandflies in China revealed viral, bacterial, and eukaryotic microbes potentially pathogenic to humans.

Phlebotomus chinensis sandfly is a neglected insect vector in China that is well-known for carrying Leishmania. Recent studies have expanded its pathogen repertoire with two novel arthropod-borne phleboviruses capable of infecting humans and animals. Despite these discoveries, our knowledge of the general pathogen diversity and overall microbiome composition of this vector species is still very limited. Here we carried out a meta-transcriptomics analysis that revealed the actively replicating/transcribing RNA viruses, DNA viruses, bacteria, and eukaryotic microbes, namely, the "total microbiome", of several sandfly populations in China. Strikingly, "microbiome" made up 1.8% of total non-ribosomal RNA and comprised more than 87 species, among which 70 were novel, including divergent members of the genera Flavivirus and of the family Trypanosomatidae. Importantly, among these microbes we were able to reveal four distinguished types of human and/or mammalian pathogens, including two phleboviruses (hedi and wuxiang viruses), one novel Spotted fever group rickettsia, as well as a member of Leishmania donovani complex, among which hedi virus and Leishmania each had > 50% pool prevalence rate and relatively high abundance levels. Our study also showed the ubiquitous presence of an endosymbiont, namely Wolbachia, although no anti-viral or anti-pathogen effects were detected based on our data. In summary, our results uncovered the much un-explored diversity of microbes harboured by sandflies in China and demonstrated that high pathogen diversity and abundance are currently present in multiple populations, implying disease potential for exposed local human population or domestic animals.

Electrosynthesis of Vertically Aligned Zinc Oxide Nanoflakes on 3D Porous Cu Foam Enables Dendrite-Free Li-Metal Anode.

Three dimensional (3D) hosts have been recognized as effective current collectors for Li metal anodes because of their physical suppression of the lithium dendrites growth. A lithiophilic surface layer on them could increase the Li metal nucleation sites, further regulating the genuine plating of Li metal. The current strategies to construct this lithiophilic layer on 3D structure is complex and not suitable for the scalable fabrication of Li metal anode. In this work, we developed a facile method to grow vertically aligned ZnO nanoflakes on the surface of 3D Cu foam through an electrochemical synthetic process, which physically suppressed the Li dendrites growth due to the unique structure during the Li plating/stripping process. Moreover, these lithiophilic flakes effectively increase the specific surface area of the anode and Li metal nucleation sites number, which reduces the local current densities, leading to the formation of a robust SEI and further suppressing the Li dendrites growth. Consequently, the performances of the symmetric Li plated Cu foam/Li cell and the Li plated Cu foam/LiFePO4 full cell have been greatly enhanced after the growth of vertically aligned ZnO nanoflakes on the Cu foam surface, including capacity, cycling stability, overpotential, and rate capability.

A collimator design method for the tomographic gamma scanning system with a fan-shaped NaI(Tl) detector array.

The detection speed of the tomographic gamma scanning (TGS) system with a detector array is faster than the single detector system. The NaI(Tl) detector is inexpensive and can work at room temperature, making it ideal for use in the TGS system with a fan-shaped detector array. The collimator of the TGS system is one of the critical elements to ensure the reconstructed image's quality. In addition to providing good detection efficiency of the detector while improving the system's spatial resolution, a proper collimator structure may also reduce cross-interference between segments. We propose a collimator design method for the TGS system with a fan-shaped NaI(Tl) detector array and combine it with the Monte Carlo method to optimize the collimator. We get the collimator aperture size and shape of the TGS system through the simulation results. Simultaneously, according to the detectors' equiangular sector arrangement limitation, we propose setting up a fan-shaped shield with adjustable depth and height at the detector collimator's front. The cross-interference between segments is effectively reduced without reducing the current segment's detection efficiency. The transmission image reconstruction shows that the collimator designed by this method can be used in the TGS system with the fan-shaped NaI(Tl) detector array.

Controllable spontaneous resolution in ultrasmall Cu-Ag bimetallic cluster ion pairs from achiral components.

Bimetallic cluster ion pairs containing a quaternary phosphonium and an ultrasmall Cu2Ag3 anionic cluster protected by thiolates: (PPh3R'')[Cu2Ag3(SR')6] (R'SH = cyclohexylthiol (CySH), R'' = Ph, 1; Me, 2; Et, 3; Pr, 4; R'SH = tert-butylthiol (tBuSH) and R'' = Ph, 5) were reported. Without any chiral source, 1 crystallizes as conglomerate crystals with homochiral packings and spontaneous resolution occurs, while four other clusters 2-5 crystallize as racemic crystals with heterochiral packings. These results indicate that racemic and homochiral crystallization in the cluster system could be controlled through fine-tuning internal achiral structural components.

Unusual Intramolecular Motion of ReH92- in K2ReH9 Crystal: Circle Dance and Three-Arm Turnstile Mechanisms Revealed by Computational Studies.

The nonahydridorhenate dianion ReH92- is a unique rhenium polyhydride complex due to its remarkably high coordination number; however, its detailed polytopal rearrangement process in either solution or crystal is so far unclear. In this work, our quantum chemical calculations have identified two previously unreported fluxional mechanisms for the ReH92- dianion in the K2ReH9 crystal: three-arm turnstile rotation and circle dance mechanism. These two polytopal rearrangements in the crystal offer an alternative interpretation to the pulse and wide-line NMR spectra (Farrar et al. J. Chem. Phys. 1969, 51, 3595). The previously postulated hindered rotation of the whole ReH92- dianion in K2ReH9 (White et al. J. Chem. Soc., Faraday Trans. 2 1972, 68, 1414) turns out to be a combination of the above-mentioned two elementary fluxional processes. In addition, our calculations have confirmed the Muetterties' D3h⇌C4v rearrangement as the intramolecular motion for the ReH92- dianion in solution.

Observation of a bcc-like framework in polyhydrido copper nanoclusters.

Cu is well-known to adopt a face-centered cubic (fcc) structure in the bulk phase. Ligand-stabilized Cu nanoclusters (NCs) with atomically precise structures are an emerging class of nanomaterials. However, it remains a great challenge to have non-fcc structured Cu NCs. In this contribution, we report the syntheses and total structure determination of six 28-nuclearity polyhydrido Cu NCs: [Cu28H16(dppp)4(RS)4(CF3CO2)8] (dppp = 1,3-bis(diphenylphosphino)propane, RSH = cyclohexylthiol, 1; tert-butylthiol, 3; and 2-thiophenethiol, 4) and [Cu28H16(dppe)4(RS)4(CH3CO2)6Cl2] (dppe = 1,2-bis(diphenylphosphino)ethane, RSH = (4-isopropyl)thiophenol, 2; 4-tert-butylbenzenethiol, 5; and 4-tert-butylbenzylmercaptan, 6). Their well-defined structures solved by X-ray single crystal diffraction reveal that these 28-Cu NCs are isostructural, and the overall metal framework is arranged as a sandwich structure with a core-shell Cu2@Cu16 unit held by two Cu5 fragments. One significant finding is that the organization of 18 Cu atoms in the Cu2@Cu16 could be regarded as an incomplete and distorted version of 3 × 2 × 2 "cutout" of the body-centered cubic (bcc) bulk phase, which was strikingly different to the fcc structure of bulk Cu. The bcc framework came as a surprise, as no bcc structures have been previously observed in Cu NCs. A comparison with the ideal bcc arrangement of 18 Cu atoms in the bcc lattice suggests that the distortion of the bcc structure results from the insertion of interstitial hydrides. The existence, number, and location of hydrides in these polyhydrido Cu NCs are established by combined experimental and DFT results. These results have significant implications for the development of high-nuclearity Cu hydride NCs with a non-fcc architecture.

Exosomes: A New Pathway for Cancer Drug Resistance.

Exosomes are extracellular vesicles (EVs) that are secreted into body fluids by multiple cell types and are enriched in bioactive molecules, although their exact contents depend on the cells of origin. Studies have shown that exosomes in the tumor microenvironment affect tumor growth, metastasis and drug resistance by mediating intercellular communication and the transport of specific molecules, although their exact mechanisms of action need to be investigated further. In this review, we have summarized current knowledge on the relationship between tumor drug resistance and exosomes, and have discussed the potential applications of exosomes as diagnostic biomarkers and therapeutic targets.

Describing Polytopal Rearrangement Processes of Octacoordinate Structures. I. Renewed Insights into Fluxionality of the Rhenium Polyhydride Complex ReH5(PPh3)2(Pyridine).

Hydride ligands of transition metal polyhydride complexes with a high coordination number are prone to fluxionality leading to interesting structural dynamics. However, the underlying polytopal rearrangement pathways have been rarely studied. Based on quantum chemical calculations carried out in this work with density functional theory and coupled-cluster theory, two new fluxional mechanisms have been identified for the rhenium polyhydride complex ReH5(PPh3)2(pyridine) to jointly account for two consecutive coalescence events in the variable-temperature NMR spectra upon heating: lateral and basal three-arm turnstile rotation. The frequently cited pseudorotation in ReH5(PPh3)2(pyridine) (Lee et al. Inorg. Chem. 1996, 35, 695) turns out to be a three-step process including two lateral three-arm turnstile steps and one basal turnstile step in between. The new fluxional mechanisms discovered in this work may also exist in other transition metal polyhydrides.