Genomic characteristics of clinical multidrug-resistant Proteus isolates from a tertiary care hospital in southwest China.

Multidrug-resistant (MDR) Proteus, especially those strains producing extended-spectrum ß-lactamases (ESBL) and carbapenemases, represents a major public health concern. In the present work, we characterized 27 MDR Proteus clinical isolates, including 23 Proteus mirabilis, three Proteus terrae, and one Proteus faecis, by whole-genome analysis. Among the 27 isolates analyzed, SXT/R391 ICEs were detected in 14 strains, and the complete sequences of nine ICEs were obtained. These ICEs share a common backbone structure but also have different gene contents in hotspots and variable regions. Among them, ICEPmiChn2826, ICEPmiChn2833, ICEPmiChn3105, and ICEPmiChn3725 contain abundant antibiotic resistance genes, including the ESBL gene bla CTX-M-65. The core gene phylogenetic analysis of ICEs showed their genetic diversity, and revealed the cryptic dissemination of them in Proteus strains from food animals and humans on a China-wide scale. One of the isolates, FZP3105, acquired an NDM-1-producing MDR plasmid, designated pNDM_FZP3105, which is a self-transmissible type 1/2 hybrid IncC plasmid. Analysis of the genetic organization showed that pNDM_FZP3105 has two novel antibiotic resistance islands bearing abundant antibiotic resistance genes, among which bla NDM-1 is located in a 9.0 kb ΔTn125 bracketed by two copies of IS26 in the same direction. In isolates FZP2936 and FZP3115, bla KPC-2 was detected on an IncN plasmid, which is identical to the previously reported pT211 in Zhejiang province of China. Besides, a MDR genomic island PmGRI1, a variant of PmGRI1-YN9 from chicken in China, was identified on their chromosome. In conclusion, this study demonstrates abundant genetic diversity of mobile genetic elements carrying antibiotic resistance genes, especially ESBL and carbapenemase genes, in clinical Proteus isolates, and highlights that the continuous monitoring on their transmission and further evolution is needed.

2D Nb3SBr7 and Ta3SBr7: Experimentally Achievable Janus Photocatalysts with Robust Coexistence of Strong Optical Absorption, Intrinsic Charge Separation, and Ultrahigh Solar-to-Hydrogen Efficiency.

Recently, two-dimensional (2D) Janus semiconductors have attracted great attention in photocatalytic applications owing to their extraordinary properties, especially the intrinsic polarization-induced spontaneous carrier separation, strong optical absorption, and ultrahigh solar-to-hydrogen (STH) efficiency. However, experimental achievable candidates for 2D intrinsic Janus semiconductors are rarely reported. Herein, based on density functional theory (DFT) calculations, we uncovered two new 2D photocatalysts, namely, Janus Nb3SBr7 and Ta3SBr7 bilayers. We revealed that both structures are highly feasible to be obtained from their bulk counterparts. Excitingly, intrinsic charge separations emerge in both structures, which are beneficial to the repression of recombinations of their photoexcited carriers. Optical absorptions of both structures can be activated in the visible and even infrared regions. Most interestingly, Nb3SBr7 and Ta3SBr7 bilayers can exhibit ultrahigh STH efficiencies of 35% and 31%, respectively, which are larger than those of most 2D Janus structures. In addition, we further found that these distinguished photocatalytic properties are rather robust and are independent of their stacking modes. Experimental feasibilities and robust coexistences of intrinsic charge separations, ultrahigh STH efficiencies, and strong absorptions endow Nb3SBr7 and Ta3SBr7 bilayers as hopeful photocatalysts for water splitting.

Inartificial Two-Dimensional Ge4Se9 Janus Structures with Appropriate Direct Band Gaps and Intrinsic Polarization Boosted Charge Separation for Photocatalytic Water Splitting.

Two-dimensional (2D) Janus structures, which are totally different from prevailing 2D structures, are more interesting for photocatalytic water splitting. Here we proposed some inartificial 2D Ge4Se9 Janus structures. Excellent photocatalytic properties are revealed: (a) Ge4Se9 structures exhibit layer-independent direct gap character with appropriate band gaps of 2.53, 2.22, 2.11, and 2.03 eV for monolayered, bilayered, triple-layered, and four-layered structures, respectively. (b) Band edge positions of these 2D structures are suitable for the driving of the evolution reaction of water splitting. (c) More importantly, owning to intrinsic electric polarization, the charge densities of the valence band maximum (VBM) and the conduction band minimum (CBM) of triple-layered and four-layered Ge4Se9 structures can be notably separated. (d) In addition, we also observed that these 2D structures can possess rather pronounced optical absorption in the visible light region. This work discloses some inartificial 2D Janus structures whose fascinating properties render them as promising photocatalysts for water splitting.

Genomic characterization of Kerstersia gyiorum SWMUKG01, an isolate from a patient with respiratory infection in China.

BACKGROUND: The Gram-negative bacterium Kerstersia gyiorum, a potential etiological agent of clinical infections, was isolated from several human patients presenting clinical symptoms. Its significance as a possible pathogen has been previously overlooked as no disease has thus far been definitively associated with this bacterium. To better understand how the organism contributes to the infectious disease, we determined the complete genomic sequence of K. gyiorum SWMUKG01, the first clinical isolate from southwest China. RESULTS: The genomic data obtained displayed a single circular chromosome of 3, 945, 801 base pairs in length, which contains 3, 441 protein-coding genes, 55 tRNA genes and 9 rRNA genes. Analysis on the full spectrum of protein coding genes for cellular structures, two-component regulatory systems and iron uptake pathways that may be important for the success of the bacterial survival, colonization and establishment in the host conferred new insights into the virulence characteristics of K. gyiorum. Phylogenomic comparisons with Alcaligenaceae species indicated that K. gyiorum SWMUKG01 had a close evolutionary relationships with Alcaligenes aquatilis and Alcaligenes faecalis. CONCLUSIONS: The comprehensive analysis presented in this work determinates for the first time a complete genome sequence of K. gyiorum, which is expected to provide useful information for subsequent studies on pathogenesis of this species.

Large Intercalation Pseudocapacitance in 2D VO2 (B): Breaking through the Kinetic Barrier.

VO2 (B) features two lithiation/delithiation processes, one of which is kinetically facile and has been commonly observed at 2.5 V versus Li/Li+ in various VO2 (B) structures. In contrast, the other process, which occurs at 2.1 V versus Li/Li+ , has only been observed at elevated temperatures due to large interaction energy barrier and extremely sluggish kinetics. Here, it is demonstrated that a rational design of atomically thin, 2D nanostructures of VO2 (B) greatly lowers the interaction energy and Li+ -diffusion barrier. Consequently, the kinetically sluggish step is successfully enabled to proceed at room temperature for the first time ever. The atomically thin 2D VO2 (B) exhibits fast charge storage kinetics and enables fully reversible uptake and removal of Li ions from VO2 (B) lattice without a phase change, resulting in exceptionally high performance. This work presents an effective strategy to speed up intrinsically sluggish processes in non-van der Waals layered materials.

Anomalous Li Storage Capability in Atomically Thin Two-Dimensional Sheets of Nonlayered MoO2.

Since the first exfoliation and identification of graphene in 2004, research on layered ultrathin two-dimensional (2D) nanomaterials has achieved remarkable progress. Realizing the special importance of 2D geometry, we demonstrate that the controlled synthesis of nonlayered nanomaterials in 2D geometry can yield some unique properties that otherwise cannot be achieved in these nonlayered systems. Herein, we report a systematic study involving theoretical and experimental approaches to evaluate the Li-ion storage capability in 2D atomic sheets of nonlayered molybdenum dioxide (MoO2). We develop a novel monomer-assisted reduction process to produce high quality 2D sheets of nonlayered MoO2. When used as lithium-ion battery (LIB) anodes, these ultrathin 2D-MoO2 electrodes demonstrate extraordinary reversible capacity, as high as 1516 mAh g-1 after 100 cycles at the current rate of 100 mA g-1 and 489 mAh g-1 after 1050 cycles at 1000 mA g-1. It is evident that these ultrathin 2D sheets did not follow the normal intercalation-cum-conversion mechanism when used as LIB anodes, which was observed for their bulk analogue. Our ex situ XPS and XRD studies reveal a Li-storage mechanism in these 2D-MoO2 sheets consisting of an intercalation reaction and the formation of metallic Li phase. In addition, the 2D-MoO2 based microsupercapacitors exhibit high areal capacitance (63.1 mF cm-2 at 0.1 mA cm-2), good rate performance (81% retention from 0.1 to 2 mA cm-2), and superior cycle stability (86% retention after 10,000 cycles). We believe that our work identifies a new pathway to make 2D nanostructures from nonlayered compounds, which results in an extremely enhanced energy storage capability.

Coexistence of Co doping and strain on arsenene and antimonene: tunable magnetism and half-metallic behavior.

Effectively modulating the magnetism of two-dimensional (2D) systems is critical for the application of magnetic nanostructures in quantum information devices. In this work, by employing density functional theory calculations, we found the coexistence of Co doping and strain can effectively control the spin states of arsenene and antimonene structures. Unstrained Co-doped arsenene (arsenene-Co) and Co-doped antimonene (antimonene-Co) structures are nonmagnetic while under a strain, the magnetic moments of both cases were abruptly increased to about 2 µ B. The emergence of magnetism can be reflected by the reduction of the interactions between Co and its neighboring atoms by the strain, which leads to the spin-splitting of Co-3d states. More importantly, we found that the transition of magnetism accompanies the modifications of the electronic properties of arsenene and antimonene so that under strain both structures can exhibit a novel half-metallic behavior. These results provide an effective pathway for the development of arsenene- and antimonene-based electronic devices by applying Co doping and strain.

A MoO2 sheet as a promising electrode material: ultrafast Li-diffusion and astonishing Li-storage capacity.

The potential of MoO2 crystal as an electrode material is reported, and nanostructural MoO2 systems, including nanoparticles, nanospheres, nanobelts and nanowires, were synthesized and proved to be advanced electrode materials. A two-dimensional (2D) geometric structure represents an extreme of surface-to-volume ratio, and thus is more suitable as an electrode material in general. Stimulated by the recent fabrication of 2D MoO2, we adopted an ab initio molecular dynamics simulation and density functional theory calculation to study the stability and electrochemical properties of a MoO2 sheet. Identified by a phonon dispersion curve and potential energy curve calculations, the MoO2 sheet proved to be dynamically and thermally stable. After lithiation, similar to most promising 2D structures, we found that a Li atom can strongly adsorb on a MoO2 sheet, and the lithiated MoO2 sheet presented excellent metallic properties. Note that, compared with most promising 2D structures, we unexpectedly revealed that the diffusion barrier of the Li atom on the MoO2 sheet was much lower and the storage capacity of the MoO2 sheet was much larger. The calculated energy barrier for the diffusion of Li on the MoO2 sheet was only 75 meV, and, due to multilayer adsorption, the theoretical capacity of the MoO2 sheet can reach up to 2513 mA h g-1. Benefiting from general properties, such as strong Li-binding and excellent conductivity, and unique phenomena, such as ultrafast diffusion capacity and astonishing storage capacity, we highlight a new promising electrode material for the Li-ion battery.

Spontaneous ripple formation in phosphorene: electronic properties and possible applications.

According to the Mermin-Wagner theorem and theory of elasticity, long-range order in two-dimensional (2D) crystals will be inevitably destroyed due to a thermal fluctuation. Thus, a 2D lattice prefers a corrugation meaning that a 2D crystal is easy to present a ripple. In this work, we, via employing ab initio molecular dynamics (AIMD) simulations, for the first time evidenced that the inherent dynamics of phosphorene would lead to a spontaneous formation of ripples at room temperature. The height of a ripple closely associates with the temperature and the width. Via density functional theory (DFT) calculations, we further demonstrated that the emergence of ripples would remarkably reduce the bandgap of phosphorene. Via the construction of the unique phosphorene structure, we finally found that such a rippled structure is expected to be used in the light-emitting field. These results give us further knowledge of phosphorene, which goes beyond the current scope of phosphorene limited to the flat lattice.

A novel anti-p21Ras scFv antibody reacting specifically with human tumour cell lines and primary tumour tissues.

BACKGROUND: The ras genes play an important role in the development and progression of human tumours. Neutralizing Ras proteins in the cytoplasm could be an effective approach to blocking ras signalling. In this study, we prepared anti-p21Ras single chain fragment variable antibody (scFv) and investigated its immunoreactivity with human tumours. METHODS: The coding sequences of H-ras, K-ras, and N-ras were separately ligated into the vector pET-28a(+). Then, recombinant expressing plasmids were induced by IPTG for p21Ras expression in E. coli. Hybridoma cell lines producing anti-p21Ras monoclonal antibodies were isolated using wildtype p21Ras proteins as immunogens. Anti-p21Ras scFv antibody was prepared from the hybridoma by the phage scFv display method. The immunoreactivity of the anti-p21Ras monoclonal antibody and the scFv antibody was identified by ELISA and immunocytochemistry. RESULTS: We prokaryotically expressed wildtype H-p21Ras, K-p21Ras and N-p21Ras and generated the hybridoma cell line KGH-R1, producing anti-p21Ras monoclonal antibodies. It was demonstrated that KGH-R1 monoclonal antibody could recognize wildtype and mutated H-p21Ras, K-p21Ras and N-p21Ras in human tumour cell lines. In all 14 types of primary human cancer tissues tested, the monoclonal antibody presented strong immunoreactivity but showed weak or negative immunoreactivity in the corresponding normal tissues. Subsequently, we prepared anti-p21Ras scFv from hybridoma KGH-R1, which showed the same immunoreactivity as the original monoclonal antibody. Sequence analysis demonstrated that the nucleotides and amino acids of the scFv exhibited an approximately 50 % difference from the anti-p21Ras scFv reported previously. CONCLUSIONS: This study presents a novel anti-p21Ras scFv antibody. Our data suggest that the scFv may be useful for ras signalling blockage and may be a potential therapeutic antibody for ras-derived tumours.

Evidencing the existence of exciting half-metallicity in two-dimensional TiCl3 and VCl3 sheets.

Half-metallicity combined with wide half-metallic gap, unique ferromagnetic character and high Curie temperature has become a key driving force to develop next-generation spintronic devices. In previous studies, such half-metallicity always occurred under certain manipulation. Here, we, via examining a series of two-dimensional transition-metal trichlorides, evidenced that TiCl3 and VCl3 sheets could display exciting half-metallicity without involving any external modification. Calculated half-metallic band-gaps for TiCl3 and VCl3 sheets are about 0.60 and 1.10 eV, respectively. Magnetic coupled calculation shows that both sheets favor the ferromagnetic order with a substantial collective character. Estimated Curie temperatures can be up to 376 and 425 K for TiCl3 and VCl3 sheets, respectively. All of these results successfully disclose two new promising two-dimensional half-metallic materials toward the application of next-generation paper-like spintronic devices.

Synthesis of Atomically Thin Boron Films on Copper Foils.

Two-dimensional boron materials have recently attracted extensive theoretical interest because of their exceptional structural complexity and remarkable physical and chemical properties. However, such 2D boron monolayers have still not been synthesized. In this report, the synthesis of atomically thin 2D γ-boron films on copper foils is achieved by chemical vapor deposition using a mixture of pure boron and boron oxide powders as the boron source and hydrogen gas as the carrier gas. Strikingly, the optical band gap of the boron film was measured to be around 2.25 eV, which is close to the value (2.07 eV) determined by first-principles calculations, suggesting that the γ-B28 monolayer is a fascinating direct band gap semiconductor. Furthermore, a strong photoluminescence emission band was observed at approximately 626 nm, which is again due to the direct band gap. This study could pave the way for applications of two-dimensional boron materials in electronic and photonic devices.

Evolution of lattice structure and chemical composition of the surface reconstruction layer in Li(1.2)Ni(0.2)Mn(0.6)O2 cathode material for lithium ion batteries.

Voltage and capacity fading of layer structured lithium and manganese rich (LMR) transition metal oxide is directly related to the structural and composition evolution of the material during the cycling of the battery. However, understanding such evolution at atomic level remains elusive. On the basis of atomic level structural imaging, elemental mapping of the pristine and cycled samples, and density functional theory calculations, it is found that accompanying the hoping of Li ions is the simultaneous migration of Ni ions toward the surface from the bulk lattice, leading to the gradual depletion of Ni in the bulk lattice and thickening of a Ni enriched surface reconstruction layer (SRL). Furthermore, Ni and Mn also exhibit concentration partitions within the thin layer of SRL in the cycled samples where Ni is almost depleted at the very surface of the SRL, indicating the preferential dissolution of Ni ions in the electrolyte. Accompanying the elemental composition evolution, significant structural evolution is also observed and identified as a sequential phase transition of C2/m → I41 → Spinel. For the first time, it is found that the surface facet terminated with pure cation/anion is more stable than that with a mixture of cation and anion. These findings firmly established how the elemental species in the lattice of LMR cathode transfer from the bulk lattice to surface layer and further into the electrolyte, clarifying the long-standing confusion and debate on the structure and chemistry of the surface layer and their correlation with the voltage fading and capacity decaying of LMR cathode. Therefore, this work provides critical insights for design of cathode materials with both high capacity and voltage stability during cycling.

Evidencing the existence of intrinsic half-metallicity and ferromagnetism in zigzag gallium sulfide nanoribbons.

The achievement of half-metallicity with ferromagnetic (FM) coupling has become a key technology for the development of one-dimensional (1D) nanoribbons for spintronic applications. Unfortunately, in previous studies, such a half-metallicity always occurs upon certain external constraints. Here we, for the first time, demonstrate, via density functional theory (DFT), that the recent experimentally realized gallium sulfide nanoribbons (GaSNRs) can display an intrinsic half-metallic character with FM coupling, raised from Ga-4s, Ga-4p and S-3p states at the Ga-dominated edge. Furthermore, the novel half-metallic behavior with FM coupling here is rather robust, especially for GaSNRs with large width and thickness, and can be sustained to the room temperature. Thus, our results accidentally disclose a new 1D spin nanomaterial, which allows us to go beyond the current scope limited to the graphene, boron nitride (BN), zinc oxide (ZnO) and molybdenum sulfide (MoS2) nanoribbons, toward more realistic spintronic applications.

Modulating the band gap of germanane nanoribbons for quantum well devices.

The effective modulation of the band gaps in nanostructures is of both fundamental and technological interest because a tunable band gap gives great flexibility in the design and optimization of nanodevices. Using density functional theory calculations, we have shown that germanane nanoribbons of various widths or under various strains can provide rich band gaps. Width- and strain-induced changes in the band gaps of germanane nanoribbons result from a reduction in quantum confinement with width and the weakening of sp(3) hybridization with strain, respectively. Both changes represent a monotonous relationship. To utilize such a monotonous change in band gap, we designed a quantum well based on germanane nanoribbons in which photoexcited electrons and holes occupy the same spatial region, resulting in a desirable light-emitting device.

Controlling magnetism of MoS2 sheets by embedding transition-metal atoms and applying strain.

Prompted by recent experimental achievement of transition metal (TM) atoms substituted in MoS2 nanostructures during growth or saturating existing vacancies (Sun et al., ACS Nano, 2013, 7, 3506; Deepak et al., J. Am. Chem. Soc., 2007, 129, 12549), we explored, via density functional theory, the magnetic properties of a series of 3d TM atoms substituted in a MoS2 sheet, and found that Mn, Fe, Co, Ni, Cu and Zn substitutions can induce magnetism in the MoS2 sheet. The localizing unpaired 3d electrons of TM atoms respond to the introduction of a magnetic moment. Depending on the species of TM atoms, the substituted MoS2 sheet can be a metal, semiconductor or half-metal. Remarkably, the applied elastic strain can be used to control the strength of the spin-splitting of TM-3d orbitals, leading to an effective manipulation of the magnetism of the TM-substituted MoS2 sheet. We found that the magnetic moment of the Mn- and Fe-substituted MoS2 sheets can monotonously increase with the increase of tensile strain, while the magnetic moment of Co-, Ni-, Cu- and Zn-substituted MoS2 sheets initially increases and then decreases with the increase of tensile strain. An instructive mechanism was proposed to qualitatively explain the variation of magnetism with elastic strain. The finding of the magnetoelastic effect here is technologically important for the fabrication of strain-driven spin devices on MoS2 nanostructures, which allows us to go beyond the current scope limited to the spin devices within graphene and BN-based nanostructures.

Electron-rich driven electrochemical solid-state amorphization in Li-Si alloys.

The physical and chemical behaviors of materials used in energy storage devices, such as lithium-ion batteries (LIBs), are mainly controlled by an electrochemical process, which normally involves insertion/extraction of ions into/from a host lattice with a concurrent flow of electrons to compensate charge balance. The fundamental physics and chemistry governing the behavior of materials in response to the ions insertion/extraction is not known. Herein, a combination of in situ lithiation experiments and large-scale ab initio molecular dynamics simulations are performed to explore the mechanisms of the electrochemically driven solid-state amorphization in Li-Si systems. We find that local electron-rich condition governs the electrochemically driven solid-state amorphization of Li-Si alloys. This discovery provides the fundamental explanation of why lithium insertion in semiconductor and insulators leads to amorphization, whereas in metals, it leads to a crystalline alloy. The present work correlates electrochemically driven reactions with ion insertion, electron transfer, lattice stability, and phase equilibrium.

Remarkable magnetism and ferromagnetic coupling in semi-sulfuretted transition-metal dichalcogenides.

Motivated by recent investigations of semi-decorated two dimensional honeycomb structures, we demonstrated, via spin-polarized molecular-dynamics simulations and density-functional-theory calculations, that semi-sulfuretted transition-metal dichalcogenides of MX type (M = V, Nb, Ta; X = S, Se, Te) are stable and display remarkable magnetism. The unpaired d electron of the transition-metal atom arising from the breakage of the M-X bond is the mechanism behind the induction of the magnetism. The remarkable magnetism of the transition-metal atoms is caused by ferromagnetic coupling due to the competitive effects of through-bond interactions and through-space interactions. This implies the existence of an infinite ferromagnetic sheet with structural integrity and magnetic homogeneity. The estimated Curie temperatures suggest that the ferromagnetism can be achieved above room temperature in the VS, VSe, VTe, NbTe and TaTe sheets. Depending on the species of the M and X atoms, the MX sheet can be a magnetic metal, magnetic semiconductor or half-metal. Furthermore, in contrary to the recently reported semi-hydrogenated and semi-fluorinated layered materials consisting of B, C, N, etc., the MX sheets with many unpaired d electrons can offer a much stronger spin polarization and possess a more stable ferromagnetic coupling, which is critical for practical nanoscale device applications.

Electronic structures and magnetic properties of MoS2 nanostructures: atomic defects, nanoholes, nanodots and antidots.

Developing approaches to effectively induce and control the magnetic states is critical to the use of magnetic nanostructures in quantum information devices but is still challenging. Here MoS2-based nanostructures including atomic defects, nanoholes, nanodots and antidots are characterized with spin-polarized density functional theory. The S-vacancy defect is more likely to form than the Mo-vacancy defect due to the form of Mo-Mo metallic bonds. Among different shaped nanoholes and nanodots, triangle ones associated with ferromagnetic characteristic are most energetically favorable, and exhibit unexpected large spin moments that scale linearly with edged length. In particular, S-terminated triangle nanodots show strong spin anisotropy around the Fermi level with a substantial collective characteristic of spin states at edges, enabling it to a desired spin-filtering structure. However, in the antidot, the net spin, coupled order and stability of spin states can be engineered by controlling type and distance of internal nanoholes. Based on the analysis of the spin coupled mechanism, a specific antidot structure, the only S-terminated antidot, was determined to exhibit a large net spin with long-range ferromagnetic coupling above room temperature. Given the recent achievement of graphene- and BN-based nanohole, nanodot and antidot structures, we believe that our calculated results are suitable for experimental verification and implementation opening a new path to explore MoS2-based magnetic nanostructures.

In situ nitrogen-doped graphene grown from polydimethylsiloxane by plasma enhanced chemical vapor deposition.

Due to its unique electronic properties and wide spectrum of promising applications, graphene has attracted much attention from scientists in various fields. Control and engineering of graphene's semiconducting properties is considered to be key to its applications in electronic devices. Here, we report a novel method to prepare in situ nitrogen-doped graphene by microwave plasma assisted chemical vapor deposition (CVD) using PDMS (polydimethylsiloxane) as a solid carbon source. Based on this approach, the concentration of nitrogen-doping can be easily controlled via the flow rate of nitrogen during the CVD process. X-ray photoelectron spectroscopy results indicated that the nitrogen atoms doped into the graphene lattice were mainly in the forms of pyridinic and pyrrolic structures. Moreover, first-principles calculations show that the incorporated nitrogen atoms can lead to p-type doping of graphene. This in situ approach provides a promising strategy to prepare graphene with controlled electronic properties.