Global epidemiology and genetic diversity of mcr-positive Klebsiella pneumoniae: A systematic review and genomic analysis.

The rapid increase of mcr-positive Klebsiella pneumoniae (K. pneumoniae) has received considerable attention and poses a major public health concern. Here, we systematically analyzed the global distribution of mcr-positive K. pneumoniae isolates based on published articles as well as publicly available genomes. Combining strain information from 78 articles and 673 K. pneumoniae genomes, a total of 1000 mcr-positive K. pneumoniae isolates were identified. We found that mcr-positive K. pneumoniae has disseminated widely worldwide, especially in Asia, with a higher diversity of sequence types (STs). These isolates were disseminated in 57 countries and were associated with 12 different hosts. Most of the isolates were found in China and were isolated from human sources. Moreover, MLST analysis showed that ST15 and ST11 accounted for the majority of mcr-positive K. pneumoniae, which deserve sustained attention in further surveillance programs. mcr-1 and mcr-9 were the dominant mcr variants in mcr-positive K. pneumoniae. Furthermore, a Genome-wide association study (GWAS) demonstrated that mcr-1- and mcr-9-producing genomes exhibited different antibiotic resistance genes (ARGs) and mobile genetic elements (MGEs), thereby indicating a distinct evolutionary path. Notably, the phylogenetic analysis suggested that certain mcr-positive K. pneumoniae genomes from various geographical areas and hosts harbored a high degree of genetic similarities (<20 SNPs), suggesting frequent cross-region and cross-host clonal transmission. Overall, our results emphasize the significance of monitoring and exploring the transmission and evolution of mcr-positive K. pneumoniae in the context of "One health".

Modulate synthesis of CeMn solid solution using various alcohols for toluene catalytic oxidation: synergistic effect of Ce-Mn and reaction mechanism.

A redox co-precipitation method was employed to synthesize CeMn homogeneous solid solutions, utilizing various alcohols as activating agents. Ethanol effectively orchestrated the precipitation of CeO2 and MnOx, promoting their co-growth. As a result, the CeMn-EA achieved 90 % toluene conversion at 218 â„ƒ (T90 =218 â„ƒ) with a weight hourly space velocity (WHSV) of 48000 ml/(g·h). It also demonstrated high adaptability to increased WHSV, suggesting its potential for industrial-scale applications. The uniform dispersion of Ce and Mn accelerated the coupling between Ce3+/Ce4+ and Mn4+/Mn3+, engineering numerous oxygen vacancies, which enhanced the activation of gas-phase oxygen and the mobility of lattice oxygen. In situ DRIFTS confirmed that toluene oxidation accommodated both Langmuir-Hinshelwood (L-H) and Mars-van Krevelen (MvK) mechanisms, with benzoate identified as a pivotal intermediate. Enhanced oxygen mobility facilitated the cleavage of the benzene ring, which was the rate-determining step. Additionally, the introduction of H2O significantly enhanced the dissociation and adsorption of toluene and facilitated the activation of gas-phase oxygen. At higher temperatures, H2O could further activate lattice oxygen engaging in toluene oxidation. ENVIRONMENTAL IMPLICATION: Volatile organic compounds (VOCs) have emerged as major air pollutants due to the changes in air pollution patterns. They can act as precursors to near-surface ozone and haze. Toluene, a typical VOC, is primarily released from anthropogenic sources and poses significant risks to human health and the environment. Ce-based catalysts have been demonstrated efficiency in toluene oxidation due to their excellent oxygen storage and release properties. This study synthesized CeMn homogeneous solid solutions utilizing various alcohols as activating agents, which possessed abundant oxygen vacancies and optimum oxygen activation capacity to oxidize toluene in time.

Global distribution and genetic characterization of blaOXA-positive plasmids in Escherichia coli.

In recent years, the emergence of blaOXA-encoding Escherichia coli (E. coli) poses a significant threat to human health. Here, we systematically analyzed the global geographic distribution and genetic characteristics of 328 blaOXA-positive E. coli plasmids based on NCBI database. Twelve blaOXA variants have been discovered, with blaOXA-1 (57.93%) being the most common, followed by blaOXA-10 (11.28%) and blaOXA-48 (10.67%). Our results suggested that blaOXA-positive E. coli plasmids were widespread in 40 countries, mainly in China, the United States, and Spain. MLST analysis showed that ST2, ST43, and ST471 were the top three host STs for blaOXA-positive plasmids, deserving continuing attention in future surveillance program. Network analysis revealed a correlation between different blaOXA variants and specific antibiotic resistance genes, such as blaOXA-1 and aac (6')-Ib-cr (95.79%), blaOXA-181 and qnrS1 (87.88%). The frequent detection of aminoglycosides-, carbapenems- and even colistin-related resistance genes in blaOXA-positive plasmids highlights their multidrug-resistant potential. Additionally, blaOXA-positive plasmids were further divided into eight clades, clade I-VIII. Each clade displayed specificity in replicon types and conjugative transfer elements. Different blaOXA variants were associated with specific plasmid lineages, such as blaOXA-1 and IncFII plasmids in clade II, and blaOXA-48 and IncL plasmids in clade I. Overall, our findings provide a comprehensive insight into blaOXA-positive plasmids in E. coli, highlighting the role of plasmids in blaOXA dissemination in E. coli.

Wet peroxide oxidation process catalyzed by Cu/Al2O3: phenol degradation and Cu2+ dissolution behavior.

Catalytic wet peroxide oxidation (CWPO) has become an important deep oxidation technology for organics removal in wastewater treatments. Supported Cu-based catalysts belong to an important type of CWPO catalyst. In this paper, two Cu catalysts, namely, Cu/Al2O3-air and Cu/Al2O3-H2 were prepared and evaluated through catalytic degradation of phenol. It was found that Cu/Al2O3-H2 had an excellent catalytic performance (TOC removal rate reaching 96%) and less metal dissolution than the Cu/Al2O3-air case. Moreover, when the organic removal rate was promoted at a higher temperature, the metal dissolution amounts was decreased. Combined with hydroxyl radical quenching experiments, a catalytic oxidation mechanism was proposed to explain the above-mentioned interesting behaviors of the Cu/Al2O3-H2 catalyst for CWPO. The catalytic test results as well as the proposed mechanism can provide better guide for design and synthesis of good CWPO catalysts.

Support Effect of Boron Nitride on the First N-H Bond Activation of NH3 on Ru Clusters.

Support effect is an important issue in heterogeneous catalysis, while the explicit role of a catalytic support is often unclear for catalytic reactions. A systematic density functional theory computational study is reported in this paper to elucidate the effect of a model boron nitride (BN) support on the first N-H bond activation step of NH3 on Run (n = 1, 2, 3) metal clusters. Geometry optimizations and energy calculations were carried out using density functional theory (DFT) calculation for intermediates and transition states from the starting materials undergoing the N-H activation process. The primary findings are summarized as follows. The involvement of the model BN support does not significantly alter the equilibrium structure of intermediates and transition states in the most favorable pathway (MFP). Moreover, the involvement of BN support decreases the free energy of activation, ΔG≠, thus improving the reaction rate constant. This improvement is more obvious at high temperatures like 673 K than low temperatures like 298 K. The BN support effect leading to the ΔG≠ decrease is most significant for the single Ru atom case among all three cases studied. Finally, the involvement of the model BN may change the spin transition behavior of the reaction system during the N-H bond activation process. All these findings provide a deeper insight into the support effect on the N-H bond activation of NH3 for the supported Ru catalyst in particular and for supported transition metal catalysts in general.

Selective Adsorptive Desulfurization with Alkaline-Earth Metal-Modified Zeolites in Oil in the Presence of Olefin.

Adsorptive desulfurization (ADS) was a hopeful method for deep desulfurization of oil in mild conditions. In this paper, based on the alkaline-earth (AE) metal-modified Y zeolite (AEY), synthesis, systematic characterization, ADS performance test, and analysis of related adsorption mechanisms were carried out. The crystal and pore structure of Y zeolite were not damaged after ion exchange of AE, while the amount of acid sites and the ratio of Lewis/Bronsted acid sites were both decreased. Although surface acid sites on zeolites were believed to be active sites for ADS, the performance test results showed that AEY adsorbents had rather good S adsorption capacity compared to NaY. Moreover, the S adsorption selectivity in the presence of hexene-1 in oil was also desirable for all AEY adsorbents. Based on these experimental results and previously proposed mechanisms for S-containing compound adsorption, a new adsorption mechanism was proposed for AEY, and this mechanism was further supported by the aid of DFT calculations. The good S-removal performance of AEY adsorbents as well as the new proposed adsorption mechanism may help people design and synthesize further improved S-compound adsorbents for ADS processes in an oil refinery.

A density functional theory study on the adsorption of different organic sulfides on boron nitride nanosheet.

The adsorption of methanethiol (MT), thiophene (T), benzothiophene (BT), dibenzothiophene (DBT) on hexagonal boron nitride (h-BN) has been investigated by the framework of the density functional theory (DFT) calculations in this work. The prefer adsorption sites and interfacial angles of different sulfur compounds on the surface of the h-BN are investigated and analyzed. The adsorption energy results indicated that the adsorption of MT (Ead ≈ -6 kcal mol-1), T (Ead ≈ -10 kcal mol-1), BT (Ead ≈ -15 kcal mol-1), and DBT (Ead ≈ -21 kcal mol-1) on monolayer h-BN is physical interaction, and the value of Ead on bilayer h-BN is more than that on monolayer h-BN 0.05%. Adsorptive conformations show that sulfides prefer to be adsorbed on center B atoms rather than N atoms. Meanwhile, thiophene and its analogues tend to be adsorbed parallel on h-BN plane. Energy decomposition, natural population analysis (NPA), and electrostatic potential (ESP) analysis used to better understand the nature of adsorption on h-BN. van der Waals force plays a dominant role in adsorption process. Due to the π-π interactions, T, BT, and DBT have larger van der Waals forces than MT and the value of adsorption energy is negative correlated to the number of benzene rings. These findings are helpful for deeper understanding the adsorptive desulfurization mechanism and help develop better adsorbents for desulfurization in the future.

Analysis of the features of 105 confirmed CRISPR loci in 487 Klebsiella variicola.

Klebsiella variicola, an emerging human pathogen, poses a threat to public health. The horizontal gene transfer (HGT) of plasmids is an important driver of the emergence of multiple antibiotic-resistant K. variicola. Clustered regularly interspersed short palindromic repeats (CRISPR) coupled with CRISPR-associated genes (CRISPR/Cas) constitute an adaptive immune system in bacteria, and can provide acquired immunity against HGT. However, the information about the CRISPR/Cas system in K. variicola is still limited. In this study, 487 genomes of K. variicola obtained from the National Center for Biotechnology Information database were used to analyze the characteristics of CRISPR/Cas systems. Approximately 21.56% of genomes (105/487) harbor at least one confirmed CRISPR array. Three types of CRISPR/Cas systems, namely the type I-E, I-E*, and IV-A systems, were identified among 105 strains. Spacer origin analysis further revealed that approximately one-third of spacers significantly match plasmids or phages, which demonstrates the implication of CRISPR/Cas systems in controlling HGT. Moreover, spacers in K. variicola tend to target mobile genetic elements from K. pneumoniae. This finding provides new evidence of the interaction of K. variicola and K. pneumoniae during their evolution. Collectively, our results provide valuable insights into the role of CRISPR/Cas systems in K. variicola.

Characterization and diversity of CRISPR/Cas systems in Klebsiella oxytoca.

CRISPR (clustered regularly interspaced short palindromic repeats)/Cas (CRISPR-associated protein) system is a crucial adaptive immune system for bacteria to resist foreign DNA infection. In this study, we investigated the prevalence and diversity of CRISPR/Cas systems in 175 Klebsiella oxytoca (K. oxytoca) strains. Specifically, 58.86% (103/175) of these strains possessed at least one confirmed CRISPR locus. Two CRISPR/Cas system types, I-F and IV-A3, were identified in 69 strains. Type I-F system was the most prevalent in this species, which correlated well with MLST. Differently, type IV-A3 system was randomly distributed. Moreover, the type IV-A3 system was separated into two subgroups, with subgroup-specific cas genes and repeat sequences. In addition, spacer origin analysis revealed that approximately one-fifth of type I-F spacers and one-third of type IV-A3 spacers had a significant match to MGEs. The phage tail tape measure protein and conjunctive transfer system protein were important targets of type I-F and IV-A3 systems in K. oxytoca, respectively. PAM sequences were inferred to be 5'-NCC-3' for type I-F, 5'-AAG-3' for subgroup IV-A3-a, and 5'-AAN-3' for subgroup IV-A3-b. Collectively, our findings will shed light on the prevalence, diversity, and functional effects of the CRISPR/Cas system in K. oxytoca.

Supported Ni Catalysts: Simple Vapor Deposition Preparation Method and Improved Catalytic Performance for Oxidative Dehydrogenation of Ethane.

Developing new methods of catalyst preparation is one of the most important tasks in the field of catalysis. A simple one-tube vapor deposition (VD) is provided in this paper for preparing the supported Ni catalyst. Ni(acac)2 was used as the Ni precursor. This preparation method was successfully applied to three types of catalytic supports, that is, Al2O3 and zeolites 5A and Hß. Varying Ni contents of less than 8 wt % can be obtained by employing different conditions. The Ni content, depending on different deposition conditions, was preliminarily explored. The catalytic performance for oxidative dehydrogenation of ethane (ODHE) was tested for the prepared Ni catalysts by the VD method. Several cases of catalytic tests showed that for the same Ni content, the VD-prepared Ni catalyst presented better performance for ODHE than the one prepared by a traditional impregnation method. Besides the improvement in catalytic performance, several advantages of our VD preparation method for catalysis are discussed.

On the mechanism of acceptorless dehydrogenation of N-heterocycles catalyzed by tBuOK: a computational study.

The catalytic acceptorless dehydrogenation (ADH) of saturated N-heterocycles has recently gained considerable attention as a promising strategy for hydrogen release from liquid organic hydrogen carriers (LOHCs). Recently, a simple tBuOK base-promoted ADH of N-heterocycles was developed by Yu et al. (Adv. Synth. Catal. 2019, 361, 3958). However, it is still open as to how the tBuOK plays a catalytic role in the ADH process. Herein, our density functional study reveals that the tBuOK catalyzes the ADH of 1,2,3,4-tetrahydroquinoline (THQ) through a quasi-metal-ligand bifunctional catalytic channel or a base-catalyzed pathway with close energy barriers. The hydride transfer in the first dehydrogenation process is determined to be the rate determining step, and the second dehydrogenation can proceed directly from 34DHQ regulated by the tBuOK. In addition, the computational results show that the cooperation of a suitable alkali metal ion with the tBuO- group is so critical that the tBuOLi and the isolated tBuO- are both inferior to tBuOK as a dehydrogenation catalyst.

Analysis of the Differential Expression and Antiviral Activity of Porcine Interferon-α In Vitro.

Porcine interferon α (poIFN-α) is a crucial cytokine that can prevent and treat viral infections. Seventeen functional porcine IFN-α subtypes were found in the porcine genome. In this study, multiple sequence alignment was performed to analyze IFN-α protein structure and function. Phylogenetic tree analysis of the poIFN gene family defined the evolutionary relationship of various subtypes. PoIFN-αs, including poIFN-α1-17, were expressed in an Escherichia coli expression system. The antiviral activities of these IFN-α proteins against vesicular stomatitis virus (VSV) and pseudorabies virus (PRV) were examined in PK-15 cells. We found that the antiviral activity of different poIFN-α molecules greatly differed as follows: the poIFN-α14 and 17 subtypes had the greatest antiviral activities against VSV and PRV in PK-15 cells, poIFN-α1, 2, 3, and 8 exhibited lower biological activities, and poIFN-α4, 5, 6, 7, 9, 10, 11, 12, 13, and 16 had minimal or no effect in the tested target cell‒virus systems. Moreover, our studies demonstrated that the antiviral activity of IFN-α was positively correlated with the induction of IFN-stimulated genes, such as 2'-5' oligoadenylate synthetase 1 (OSA1), interferon-stimulated gene 15 (ISG15), myxoma resistance protein 1 (Mx1), and protein kinase R (PKR). Thus, our experimental results provide important information about the antiviral functions and mechanism of poIFN-α.

Genomic Insights into CRISPR-Harboring Plasmids in the Klebsiella Genus: Distribution, Backbone Structures, Antibiotic Resistance, and Virulence Determinant Profiles.

CRISPR systems are often encoded by many prokaryotes as adaptive defense against mobile genetic elements (MGEs), but several MGEs also recruit CRISPR components to perform additional biological functions. Type IV-A systems are identified in Klebsiella plasmids, yet the distribution, characterization, and role of these plasmids carrying CRISPR systems in the whole Klebsiella genus remain unclear. Here, we performed large-scale comparative analysis of these plasmids using publicly available plasmid genomes. CRISPR-harboring plasmids were mainly distributed in Klebsiella pneumoniae (9.09%), covering 19.23% of sequence types, but sparse in Klebsiella species outside Klebsiella pneumoniae (3.92%). Plasmid genome comparison reiterated that these plasmids often carried the cointegrates of IncFIB and IncHI1B replicons, occasionally linked to other replicons, such as IncFIA, IncFII, IncR, IncQ, and IncU. Comparative genome analysis showed that CRISPR-carrying Klebsiella plasmids shared a conserved pNDM-MAR-like conjugation module as their backbones and served as an important vector for the accretion of antibiotic resistance genes (ARGs) and even virulence genes (VGs). Moreover, compared with CRISPR-negative IncFIB/IncHIB plasmids, CRISPR-positive IncFIB/IncHIB plasmids displayed high divergences in terms of ARGs, VGs, GC content, plasmid length, and backbone structures, suggesting their divergent evolutionary paths. The network analysis revealed that CRISPR-positive plasmids yielded fierce competitions with other plasmid types, especially conjugative plasmids, thereby affecting the dynamics of plasmid transmission. Overall, our study provides valuable insights into the role of CRISPR-positive plasmids in the spread of ARGs and VGs in Klebsiella genus.

Sulfone-Decorated Conjugated Organic Polymers Activate Oxygen for Photocatalytic Methane Conversion.

Oxidizing CH4 into liquid products with O2 under mild conditions still mainly relies on metal catalysis. We prepared a series of sulfone-modified conjugated organic polymers and found that the catalyst with proper SVI content (0.10) could drive O2 →H2 O2 →⋅OH to oxidize CH4 into CH3 OH and HCOOH directly and efficiently at room temperature under light irradiation. Experimental results showed that after 4 h reaction, decomposition rate and residual amounts of H2 O2 were 81.21 % and 4.83 mmol gcat -1 respectively, and CH4 conversion rate was 22.81 %. Mechanism studies revealed that illumination could induce the homolytic dissociation of S=O bonds on catalyst to produce oxygen and sulfur radicals, where the ⋅O could adsorb and activate CH4 , and the ⋅S could supply electrons for 1 O2 to generate H2 O2 and then for decomposing the H2 O2 into ⋅OH timely to oxidize CH4 . This research provided a novel organic catalysis approach for oxygen activation and utilization.

Mechanistic Insights into Visible-Light-Driven Dearomative Fluoroalkylation Mediated by an Electron Donor-Acceptor Complex.

Electron donor-acceptor (EDA) complex photochemistry has become a burgeoning topic in the synthetic radical chemistry mediated by visible light; however, the theoretical insights into the reaction mechanisms are limited. Herein, accurate electronic structure calculations at the CASPT2//CASSCF/PCM level of theory were performed to investigate the paradigm example of EDA complex-enabled photoreaction for visible-light-driven dearomative perfluoroalkylation of ß-naphthol. The excitation energy levels of the EDA complex are controlled by noncovalent interactions because the photoinduced intermolecular charge is enhanced when the noncovalent interaction becomes weaker, leading to the broad spectra ranging from UVA (<380 nm) to visible light (>500 nm). The competitiveness of the radical-radical coupling over the radical chain pathway is also regulated due to the tunable radical concentrations varying the excitation wavelength.

Vapor Deposition-Prepared MIL-100(Cr)- and MIL-101(Cr)-Supported Iron Catalysts for Effectively Removing Organic Pollutants from Water.

Metal organic framework (MOF)-supported Fe catalysts belong to an important class of catalysts used for the advanced oxidation of organic pollutants in water. The successful preparation of the Fe/MIL-100(Cr) and Fe/MIL-101(Cr) catalysts in this work reinforced that a recently established carrier-gas free vapor deposition method can be a general one for preparing Fe/MOF catalysts. The Fe loading was in the range of 7.8-27.2 wt % on Fe/MIL-101(Cr) at a deposition temperature of 110-150 °C, and it was only 4.35 wt % on Fe/MIL-100(Cr) at 110 °C in comparison. The results obtained from the characterization using the N2-isotherm and EDX mapping showed that the Fe components resided uniformly within the pore of the MOF supports. Both of Fe/MIL-100(Cr) and Fe/MIL-101(Cr) were rather effective for the catalytic removal of aniline from water with Fenton oxidation. Fe/MIL-100(Cr) can effectively remove the total organic carbon (TOC) of the aniline solutions, while Fe/MIL-101(Cr) had a lower TOC removal efficiency. Both of the Fe/MIL-100(Cr) and Fe/MIL-101(Cr) catalysts showed good stability in the crystalline form compared to the previously prepared Fe/UiO-66 catalyst, implicating that they can be potentially more useful than Fe/UiO-66 for treating organic pollutants in water.

Supported Pt-Cu bimetallic catalysts: preparation and synergic effects in their catalytic oxidative degradation of aniline.

Catalytic Fenton oxidation is an effective way to remove organic pollutants in water, and the performance of the catalyst is a key issue for the competiveness of this method. In this work, various supported bimetallic Pt-Cu catalysts were prepared by different impregnation methods and their performances for catalytic Fenton oxidation of aniline in water were investigated. In the different impregnation methods employed, factors including the reduction method of the metal precursor, type of catalytic support, and loading of metal were investigated. The effect of different reduction methods on actual loadings of the active components on the supported Pt-Cu catalysts showed the order of (i) H2 reduction > (ii) liquid phase methanal reduction. Meanwhile, compared with the monometallic catalysts, the Pt-Cu alloy phase (mainly in the form of PtCu3) was generated and the specific surface area was significantly reduced for the bimetallic catalysts. In the process of Fenton catalytic oxidation of aniline, it was found that most of the prepared catalysts had a certain catalytic activity for H2O2 accompanied with aniline degradation. It was found that Pt0.5Cu1.5/AC (where AC denotes activated carbon) exhibited superb catalytic activity compared with all other prepared catalysts. In particular, aniline was almost completely mineralized in a neutral solution (500 mg L-1 aniline, 0.098 mol L-1 H2O2) after 60 min at 50 °C using Pt-Cu/AC (Pt: 0.5%, Cu: 1.5%). The characterization results showed that the Pt and Cu components were rather evenly distributed on the AC support for this catalyst. More importantly, there was an obvious synergic effect on the supported bimetallic catalyst between the Pt and Cu components for the catalytic oxidation of aniline.

Mechanistic insights into the C-H activation of methane mediated by the unsupported and silica-supported VO2OH and CrOOH: a DFT study.

The direct activation and conversion of methane has been a topic of interest in both academia and industry for several decades. Deep understanding of the corresponding mechanism and reactivity mediated by diverse catalytic clusters, as well as the supporting materials, is still highly desired. In this work, the regulation mechanism of C-H bond activation of methane, mediated by the closed-shell VO2OH, the open-shell CrOOH, and their silica supported clusters, has been investigated by density functional theory (DFT) calculations. The hydrogen-atom transfer (HAT) reaction towards methane C-H bond activation is more feasible when mediated by the unsupported/silica-supported CrOOH clusters versus the VO2OH clusters, due to the intrinsic spin density located on the terminal Ot atom. The proton-coupled electron transfer (PCET) pathways are regulated by both the nucleophilicity of the Ot site and the electrophilicity of the metal center, which show no obvious difference in energy consumption among the four reactions examined. Moreover, the introduction of a silica support can lead to subtle influences on the intermolecular interaction between the CH4 molecule and the catalyst cluster, as well as the thermodynamics of the methane C-H activation.

Unraveling How the H2 Treatment Helps Improve the Performances of Cu and Ag Loaded Y Zeolites for Adsorptive Desulfurization.

This work seeks for a better understanding on how the gas treatment process affected the structure of metal loaded zeolite Y (MY, M = Ag, Cu) adsorbants and how the structural changes affected the performances of the adsorbents for adsorptive desulfurization. A series of characterization tools including solid-state nuclear magnetic resonance were employed. Compared to the N2 treatment, the H2 treatment on the MY adsorbents led to the reduction of the loaded M components to their metallic state and, consequently, brought several structural changes to the zeolitic framework. The structural changes brought by the H2 treatment can be accounted for the decreased Brönsted acidity over the Lewis acidity of the adsorbents and thus helped in improving their adsorption capacity. This paper provides new insights on how the zeolitic framework changes affected the sulfur adsorption capacity of MY, which is helpful for designing better adsorbents for sulfur removal from oil.

UiO-66-supported Fe catalyst: a vapour deposition preparation method and its superior catalytic performance for removal of organic pollutants in water.

A vapour deposition (VD) method was established for preparation of the UiO-66-supported Fe (Fe/UiO-66) catalyst, which provided the first case of the metal-organic framework (MOF)-supported Fe catalyst prepared by using the vapour-based method. The Fe loading was around 7.0-8.5 wt% under the present preparation conditions. The crystal structure of UiO-66 was not obviously influenced by the Fe loading, while the surface area significantly decreased, implicating most of the Fe components resided in the pores on UiO-66. The results for the methyl orange (MO) removal tests showed that MO in aqueous solution can be removed by UiO-66 by adsorption, and in contrast, it can be oxidized by H2O2 with the catalysis of Fe/UiO-66. Further catalytic tests showed that Fe/UiO-66 was rather effective to catalyse the oxidation of benzene derivatives like aniline in water in terms of chemical oxygen demand (COD) removal efficiency. The catalytic test results for Fe/UiO-66 were compared to those of Fe/Al2O3 with the same Fe loading and to the catalysts reported in the literature. This paper provides a general strategy for VD preparation of MOF-supported Fe catalyst on the one hand, and new catalysts for removing organic pollutants from water, on the other hand.