Selective Conversion of Cyclohexene to 2‑Methoxycyclohexanol over Molybdenum Oxide on Beta Zeolite

Selective transformation of olefins is an important route to produce cyclic monoether glycol products, but the current catalysts still suffer from insufficient activity, selectivity, and durability. Herein, we reported that molybdenum oxide on siliceous beta zeolite was highly efficient for the selective conversion of cyclohexene with a trans-2-methoxycyclohexanol yield as high as 95% in the presence of methanol and tert-butyl hydroperoxide as an oxidant. This reaction included the epoxidation of cyclohexene and subsequent solvolysis. Mechanistic studies revealed that the siliceous beta zeolite benefited the formation of abundant monomeric MoOx species, which was efficient for both the epoxidation of cyclohexene and subsequent solvolysis. Furthermore, this catalyst was also active for the conversion of other olefins, achieving the corresponding β-alkoxyalcohols

Image_1_Characterization of two multidrug-resistant Klebsiella pneumoniae harboring tigecycline-resistant gene tet(X4) in China.TIF

ObjectivesTigecycline is recognized as one of the last-line antibiotics to treat serious bacterial infection caused by carbapenem-resistant Klebsiella pneumoniae (CRKP). The plasmid-borne gene tet(X4) mediates high resistance to tigecycline. However, the prevalence and genetic context of tet(X4) in K. pneumoniae from various sources are not fully understood. Here, we investigated the prevalence of tet(X4)-positive K. pneumoniae and characterized the genetic context of tet(X4)-bearing plasmids in K. pneumoniae isolates.MethodsPolymerase chain reaction (PCR) was used to detect the tet(X4) gene. The transferability of the tet(X4)-carrying plasmids was tested by conjugation assays. The Galleria mellonella infection model was used to test virulence of tet(X4)-positive strains. Whole-genome sequencing and genome-wide analysis were performed to identify the antimicrobial resistance and the virulence genes, and to clarify the genetic characteristics of the tet(X4)-positive isolates.ResultsAmong 921 samples, we identified two tet(X4)-positive K. pneumoniae strains collected from nasal swabs of two pigs (0.22%, 2/921). The two tet(X4)-positive isolates exhibited high minimum inhibitory concentrations to tigecycline (32–256 mg/L) and tetracycline (256 mg/L). The plasmids carrying the tet(X4) gene can transfer from the donor strain K. pneumoniae to the recipient strain Escherichia coli J53. Genetic analysis of the complete sequence of two tet(X4)-carrying plasmids pTKPN_3-186k-tetX4 and pTKPN_8-216k-tetX4 disclosed that the tet(X4) gene was flanked by delta ISCR2 and IS1R, which may mediate the transmission of the tet(X4) gene.ConclusionThe prevalence of tet(X4)-positive K. pneumoniae among different sources was low. ISCR2 and IS1R may contribute to the horizontal transfer of tet(X4) gene. Effective measures should be taken to prevent the transmission of tet(X4)-producing K. pneumoniae in humans or animals.</p

Data_Sheet_1_Characterization of two multidrug-resistant Klebsiella pneumoniae harboring tigecycline-resistant gene tet(X4) in China.docx

ObjectivesTigecycline is recognized as one of the last-line antibiotics to treat serious bacterial infection caused by carbapenem-resistant Klebsiella pneumoniae (CRKP). The plasmid-borne gene tet(X4) mediates high resistance to tigecycline. However, the prevalence and genetic context of tet(X4) in K. pneumoniae from various sources are not fully understood. Here, we investigated the prevalence of tet(X4)-positive K. pneumoniae and characterized the genetic context of tet(X4)-bearing plasmids in K. pneumoniae isolates.MethodsPolymerase chain reaction (PCR) was used to detect the tet(X4) gene. The transferability of the tet(X4)-carrying plasmids was tested by conjugation assays. The Galleria mellonella infection model was used to test virulence of tet(X4)-positive strains. Whole-genome sequencing and genome-wide analysis were performed to identify the antimicrobial resistance and the virulence genes, and to clarify the genetic characteristics of the tet(X4)-positive isolates.ResultsAmong 921 samples, we identified two tet(X4)-positive K. pneumoniae strains collected from nasal swabs of two pigs (0.22%, 2/921). The two tet(X4)-positive isolates exhibited high minimum inhibitory concentrations to tigecycline (32–256 mg/L) and tetracycline (256 mg/L). The plasmids carrying the tet(X4) gene can transfer from the donor strain K. pneumoniae to the recipient strain Escherichia coli J53. Genetic analysis of the complete sequence of two tet(X4)-carrying plasmids pTKPN_3-186k-tetX4 and pTKPN_8-216k-tetX4 disclosed that the tet(X4) gene was flanked by delta ISCR2 and IS1R, which may mediate the transmission of the tet(X4) gene.ConclusionThe prevalence of tet(X4)-positive K. pneumoniae among different sources was low. ISCR2 and IS1R may contribute to the horizontal transfer of tet(X4) gene. Effective measures should be taken to prevent the transmission of tet(X4)-producing K. pneumoniae in humans or animals.</p

Image_2_Characterization of two multidrug-resistant Klebsiella pneumoniae harboring tigecycline-resistant gene tet(X4) in China.TIF

ObjectivesTigecycline is recognized as one of the last-line antibiotics to treat serious bacterial infection caused by carbapenem-resistant Klebsiella pneumoniae (CRKP). The plasmid-borne gene tet(X4) mediates high resistance to tigecycline. However, the prevalence and genetic context of tet(X4) in K. pneumoniae from various sources are not fully understood. Here, we investigated the prevalence of tet(X4)-positive K. pneumoniae and characterized the genetic context of tet(X4)-bearing plasmids in K. pneumoniae isolates.MethodsPolymerase chain reaction (PCR) was used to detect the tet(X4) gene. The transferability of the tet(X4)-carrying plasmids was tested by conjugation assays. The Galleria mellonella infection model was used to test virulence of tet(X4)-positive strains. Whole-genome sequencing and genome-wide analysis were performed to identify the antimicrobial resistance and the virulence genes, and to clarify the genetic characteristics of the tet(X4)-positive isolates.ResultsAmong 921 samples, we identified two tet(X4)-positive K. pneumoniae strains collected from nasal swabs of two pigs (0.22%, 2/921). The two tet(X4)-positive isolates exhibited high minimum inhibitory concentrations to tigecycline (32–256 mg/L) and tetracycline (256 mg/L). The plasmids carrying the tet(X4) gene can transfer from the donor strain K. pneumoniae to the recipient strain Escherichia coli J53. Genetic analysis of the complete sequence of two tet(X4)-carrying plasmids pTKPN_3-186k-tetX4 and pTKPN_8-216k-tetX4 disclosed that the tet(X4) gene was flanked by delta ISCR2 and IS1R, which may mediate the transmission of the tet(X4) gene.ConclusionThe prevalence of tet(X4)-positive K. pneumoniae among different sources was low. ISCR2 and IS1R may contribute to the horizontal transfer of tet(X4) gene. Effective measures should be taken to prevent the transmission of tet(X4)-producing K. pneumoniae in humans or animals.</p

Two superconductor-insulator phase transitions in the spinel oxide Li_1±xTi₂ O_4-δ induced by ionic liquid gating

The associations between emergent physical phenomena (e.g., superconductivity) and orbital, charge, and spin degrees of freedom of 3d electrons are intriguing in transition metal compounds. Here, we successfully manipulate the superconductivity of spinel oxide Li1±xTi2O4-δ (LTO) by ionic liquid gating. A dome-shaped superconducting phase diagram is established, where two insulating phases are disclosed both in heavily electron-doping and hole-doping regions. The superconductor-insulator transition (SIT) in the hole-doping region can be attributed to the loss of Ti valence electrons. In the electron-doping region, LTO exhibits an unexpected SIT instead of a metallic behavior despite an increase in carrier density. Furthermore, a thermal hysteresis is observed in the normal state resistance curve, suggesting a first-order phase transition. We speculate that the SIT and the thermal hysteresis stem from the enhanced 3d electron correlations and the formation of orbital ordering by comparing the transport and structural results of LTO with the other spinel oxide superconductor MgTi2O4 (MTO), as well as analyzing the electronic structure by first-principles calculations. Further comprehension of the detailed interplay between superconductivity and orbital ordering would contribute to the revealing of unconventional superconducting pairing mechanism

Supplementary information files for Two superconductor-insulator phase transitions in the spinel oxide Li_1±xTi₂ O_4-δ induced by ionic liquid gating

Supplementary files for article Two superconductor-insulator phase transitions in the spinel oxide Li1±xTi2 O4-δ induced by ionic liquid gating. The associations between emergent physical phenomena (e.g., superconductivity) and orbital, charge, and spin degrees of freedom of 3d electrons are intriguing in transition metal compounds. Here, we successfully manipulate the superconductivity of spinel oxide Li1±xTi2O4-δ (LTO) by ionic liquid gating. A dome-shaped superconducting phase diagram is established, where two insulating phases are disclosed both in heavily electron-doping and hole-doping regions. The superconductor-insulator transition (SIT) in the hole-doping region can be attributed to the loss of Ti valence electrons. In the electron-doping region, LTO exhibits an unexpected SIT instead of a metallic behavior despite an increase in carrier density. Furthermore, a thermal hysteresis is observed in the normal state resistance curve, suggesting a first-order phase transition. We speculate that the SIT and the thermal hysteresis stem from the enhanced 3d electron correlations and the formation of orbital ordering by comparing the transport and structural results of LTO with the other spinel oxide superconductor MgTi2O4 (MTO), as well as analyzing the electronic structure by first-principles calculations. Further comprehension of the detailed interplay between superconductivity and orbital ordering would contribute to the revealing of unconventional superconducting pairing mechanism

A selective control of volatile and non-volatile superconductivity in an insulating copper oxide via ionic liquid gating

© 2020 Science China Press Manipulating the superconducting states of high transition temperature (high-Tc) cuprate superconductors in an efficient and reliable way is of great importance for their applications in next-generation electronics. Here, employing ionic liquid gating, a selective control of volatile and non-volatile superconductivity is achieved in pristine insulating Pr2CuO4±δ (PCO) films, based on two distinct mechanisms. Firstly, with positive electric fields, the film can be reversibly switched between superconducting and non-superconducting states, attributed to the carrier doping effect. Secondly, the film becomes more resistive by applying negative bias voltage up to − 4 V, but strikingly, a non-volatile superconductivity is achieved once the gate voltage is removed. Such phenomenon represents a distinctive route of manipulating superconductivity in PCO, resulting from the doping healing of oxygen vacancies in copper-oxygen planes as unravelled by high-resolution scanning transmission electron microscope and in situ X-ray diffraction experiments. The effective manipulation of volatile/non-volatile superconductivity in the same parent cuprate brings more functionalities to superconducting electronics, as well as supplies flexible samples for investigating the nature of quantum phase transitions in high-Tc superconductors