Separating water isotopologues using diffusion-regulatory porous materials.

The discovery of a method to separate isotopologues, molecular entities that differ in only isotopic composition1, is fundamentally and technologically essential but remains challenging2,3. Water isotopologues, which are very important in biological processes, industry, medical care, etc. are among the most difficult isotopologue pairs to separate because of their very similar physicochemical properties and chemical exchange equilibrium. Herein, we report efficient separation of water isotopologues at room temperature by constructing two porous coordination polymers (PCPs, or metal-organic frameworks) in which flip-flop molecular motions within the frameworks provide diffusion-regulatory functionality. Guest traffic is regulated by the local motions of dynamic gates on contracted pore apertures, thereby amplifying the slight differences in the diffusion rates of water isotopologues. Significant temperature-responsive adsorption occurs on both PCPs: H2O vapour is preferentially adsorbed into the PCPs, with substantially increased uptake compared to that of D2O vapour, facilitating kinetics-based vapour separation of H2O/HDO/D2O ternary mixtures with high H2O separation factors of around 210 at room temperature.

Controlling Guest Diffusion by Local Dynamic Motion in Soft Porous Crystals to Separate Water Isotopologues and Similar Gases.

ConspectusThe precise and effective separation of similar mixtures is one of the fundamental issues and essential tasks in chemical research. In the field of gas/vapor separation, the size difference among the molecular pairs/isomers of light hydrocarbons and aromatic compounds is generally 0.3-0.5 Å, and the boiling-point difference is generally 6-15 K. These are necessary industrial raw materials and have great separation demands. Still, their separation mainly relies on energy-intensive distillation technology. On the other hand, remarkably similar substances such as oxygen/argon and isotopologues usually exhibit size differences of only 0-0.07 Å and boiling-point differences of only 1-3 K. Although their industrial separation can be realized, their efficiency is considerably low. Therefore, effectively separating remarkably similar mixtures is crucial in fundamental chemistry and industry, but it remains a significant challenge. Porous coordination polymers (PCPs) or metal-organic frameworks (MOFs) are emerging materials platforms for designing adsorbents for separating similar mixtures. However, the reported PCPs did not work well for separating remarkably similar substances. The framework structures of the mainstream PCPs remain unchanged (rigid) or significantly change (globally flexible) upon adsorption. However, rigid and globally flexible PCPs find controlling the pore aperture in subangstrom precision challenging, a prerequisite for distinguishing remarkably similar substances. Thus, novel mechanisms and materials design principles are urgently needed to realize PCPs-based adsorptive separation of remarkably similar mixtures.To confront the obstacles in separating remarkably similar mixtures, our group started contributing to this field in 2017. We employed locally flexible PCPs as the materials designing platform, whose local motions of the side substituent groups potentially regulate the pore apertures to design and control the gas/vapor diffusion in PCPs. Specifically, we encoded dynamic flipping molecular motions into the diffusion-regulatory gate functionality. The ligands were designed by integrating carboxylic coordination groups with nonplanar fused-ring moieties, with the latter moieties exhibiting flipping motion around their equilibrium positions with small energy increases. Such local motions of ligands lead to the dynamic opening and blocking of PCP channels, thus termed flipping dynamic crystals (FDCs). FDCs feature distinctive temperature-responsive adsorption behaviors due to the competition of thermodynamics and kinetics under diffusion regulation, enabling differentiation of remarkably similar mixtures by each gate-admission temperature much higher than the boiling-point temperature of each component. Even when the molecular sizes are the same in the water isotopologue mixtures, FDCs can separate each isotopologue by amplifying their diffusion-rate differences. Finally, by combining the thermodynamic and kinetic factors, FDCs achieve temperature-switched recognition of CO2/C2H2 and diffusion-rate sieving of C3H6/C3H8. Therefore, our work provides a platform for designing locally flexible PCPs by introducing subangstrom precision in flexibility. This opens up the feasibility of separating remarkably similar mixtures on scientific principles. In this Account, we summarize our above ongoing research contributions, including (i) the design of flipping ligands and FDCs, (ii) the characterization of flipping motions, (iii) the gas/isotopologue sorption behaviors, and (iv) the separation of gases and isotopologues. Overall, our studies offer a new aspect of soft porous crystals and provide future opportunities for relevant researchers in this field.

Computer-aided nanodrug discovery: recent progress and future prospects.

Nanodrugs, which utilise nanomaterials in disease prevention and therapy, have attracted considerable interest since their initial conceptualisation in the 1990s. Substantial efforts have been made to develop nanodrugs for overcoming the limitations of conventional drugs, such as low targeting efficacy, high dosage and toxicity, and potential drug resistance. Despite the significant progress that has been made in nanodrug discovery, the precise design or screening of nanomaterials with desired biomedical functions prior to experimentation remains a significant challenge. This is particularly the case with regard to personalised precision nanodrugs, which require the simultaneous optimisation of the structures, compositions, and surface functionalities of nanodrugs. The development of powerful computer clusters and algorithms has made it possible to overcome this challenge through in silico methods, which provide a comprehensive understanding of the medical functions of nanodrugs in relation to their physicochemical properties. In addition, machine learning techniques have been widely employed in nanodrug research, significantly accelerating the understanding of bio-nano interactions and the development of nanodrugs. This review will present a summary of the computational advances in nanodrug discovery, focusing on the understanding of how the key interfacial interactions, namely, surface adsorption, supramolecular recognition, surface catalysis, and chemical conversion, affect the therapeutic efficacy of nanodrugs. Furthermore, this review will discuss the challenges and opportunities in computer-aided nanodrug discovery, with particular emphasis on the integrated "computation + machine learning + experimentation" strategy that can potentially accelerate the discovery of precision nanodrugs.

Proteomics of Serum Samples for the Exploration of the Pathological Mechanism of Obstetric Antiphospholipid Syndrome.

Obstetric antiphospholipid syndrome (OAPS) is a multisystem disorder characterized by thrombosis or recurrent fetal loss. In this study, we aim to explore the pathological mechanism of OAPS. Herein, we carried out data-independent acquisition (DIA) mass spectrometry quantitative proteomic analysis of serum samples from OAPS patients and healthy controls. A set of 93 differentially expressed proteins was identified, including 75 upregulated and 18 downregulated proteins compared with the levels in controls. Those proteins are enriched in KEGG pathways related to autoimmune diseases, allergic diseases, and pathogen infection. Interestingly, metabolic pathways such as fatty acid degradation and type I diabetes were enriched, indicating that OAPS is metabolic disease related. The significantly increased triglyceride also supported this idea. The differentially expressed proteins insulin-like growth factor-binding protein-1 (IGFBP-1), C-reactive protein (CRP), and ferritin light chain (FTL) were validated by ELISA. Our study presented a deep serum proteomics of OAPS and advanced our understanding of OAPS pathogenesis.

ST218 Klebsiella pneumoniae became a high-risk clone for multidrug resistance and hypervirulence.

BACKGROUND: The occurrence of multidrug-resistant and hypervirulent Klebsiella pneumoniae (MDR-hvKp) worldwide poses a great challenge for public health. Few studies have focused on ST218 MDR-hvKp. METHODS: Retrospective genomic surveillance was conducted at the Peking University Third Hospital from 2017 and clinical information was obtained. To understand genomic and microbiological characteristics, antimicrobial susceptibility testing, plasmid conjugation and stability, biofilm formation, serum killing, growth curves and whole-genome sequencing were performed. We also assessed the clinical and microbiological characteristics of ST218 compared with ST23. RESULTS: A total of eleven ST218 Kp isolates were included. The most common infection type was lower respiratory tract infection (72.7%, 8/11) in our hospital, whereas ST23 hvKp (72.7%, 8/11) was closely associated with bloodstream infection. Notably, nosocomial infections caused by ST218 (54.5%, 6/11) was slightly higher than ST23 (36.4%, 4/11). All of the ST218 and ST23 strains presented with the virulence genes combination of iucA + iroB + peg344 + rmpA + rmpA2. Interestingly, the virulence score of ST218 was lower than ST23, whereas one ST218 strain (pPEKP3107) exhibited resistance to carbapenems, cephalosporins, ß-lactamase/inhibitors and quinolones and harbored an ~ 59-kb IncN type MDR plasmid carrying resistance genes including blaNDM-1, dfrA14 and qnrS1. Importantly, blaNDM-1 and qnrS1 were flanked with IS26 located within the plasmid that could successfully transfer into E. coli J53. Additionally, PEKP2044 harbored an ~ 41-kb resistance plasmid located within tetA indicating resistance to doxycycline. CONCLUSION: The emergence of blaNDM-1 revealed that there is great potential for ST218 Kp to become a high-risk clone for MDR-hvKp, indicating the urgent need for enhanced genomic surveillance.

RACK1 and NEK7 mediate GSDMD-dependent macrophage pyroptosis upon Streptococcus suis infection.

Streptococcus suis serotype 2 (SS2) is an important zoonotic pathogen that induces an NLRP3-dependent cytokine storm. NLRP3 inflammasome activation triggers not only an inflammatory response but also pyroptosis. However, the exact mechanism underlying S. suis-induced macrophage pyroptosis is not clear. Our results showed that SS2 induced the expression of pyroptosis-associated factors, including lactate dehydrogenase (LDH) release, propidium iodide (PI) uptake and GSDMD-N expression, as well as NLRP3 inflammasome activation and IL-1ß secretion. However, GSDMD deficiency and NLRP3 inhibition using MCC950 attenuated the SS2-induced expression of pyroptosis-associated factors, suggesting that SS2 induces NLRP3-GSDMD-dependent pyroptosis. Furthermore, RACK1 knockdown also reduced the expression of pyroptosis-associated factors. In addition, RACK1 knockdown downregulated the expression of NLRP3 and Pro-IL-1ß as well as the phosphorylation of P65. Surprisingly, the interaction between RACK1 and P65 was detected by co-immunoprecipitation, indicating that RACK1 induces macrophage pyroptosis by mediating the phosphorylation of P65 to promote the transcription of NLRP3 and pro-IL-1ß. Similarly, NEK7 knockdown decreased the expression of pyroptosis-associated factors and ASC oligomerization. Moreover, the results of co-immunoprecipitation revealed the interaction of NEK7-RACK1-NLRP3 during SS2 infection, demonstrating that NEK7 mediates SS2-induced pyroptosis via the regulation of NLRP3 inflammasome assembly and activation. These results demonstrate the important role of RACK1 and NEK7 in SS2-induced pyroptosis. Our study provides new insight into SS2-induced cell death.

Application of Second-Generation Sequencing Technology in Lower Respiratory Tract Infection.

BACKGROUND: Lower respiratory tract infection (LRTI) has long been an important threat to people's life and health, so the rapid diagnosis of LRTI is of great significance in clinical treatment. In recent years, the development of the sequencing technology provides a new direction for the rapid diagnosis of LRTI. In this review, the advantages and disadvantages of second-generation sequencing techniques represented by metagenomics next-generation sequencing (mNGS) and droplet digital polymerase chain reaction (ddPCR) in LRTI were reviewed. Furthermore, it offers insights into the future trajectory of this technology, highlighting its potential to revolutionise the field of respiratory infection diagnostics. OBJECTIVE: This review summarises developments in mechanistic research of second-generation sequencing technology their relationship with clinical practice, providing insights for future research. METHODS: Authors conducted a search on PubMed and Web of Science using the professional terms 'Lower respiratory tract infection' and 'droplet digital polymerase chain reaction' and 'metagenomics next generation sequencing'. The obtained literature was then roughly categorised based on their research content. Similar studies were grouped into the same sections, and further searches were conducted based on the keywords of each section. RESULTS: Different studies discussed the application of second-generation sequencing technology in LRTI from different angles, including the detection of pathogens of LRTI by mNGS and ddPCR, the prediction ability of drug-resistant bacteria, and comparison with traditional methods. We try to analyse the advantages and disadvantages of the second-generation sequencing technology by combing the research results of mNGS and ddPCR. In addition, the development direction of the second-generation sequencing technology is prospected.

Outcomes of partial pulpotomy in permanent molars of children with irreversible pulpitis: A prospective cohort study.

BACKGROUND: Vital pulp therapy is gaining traction in dental practice, especially for young patients. AIM: To evaluate the outcomes of partial pulpotomy in permanent molars of children diagnosed with irreversible pulpitis (IP) using iRoot BP Plus. DESIGN: A total of 94 permanent molars in 88 patients, aged 6-15 years, with symptoms of IP, were treated with partial pulpotomy, using iRoot BP Plus as the pulp capping agent. The treated teeth underwent clinical and radiographic assessments at 1, 6, 12, 18, and 24 months postoperative. The outcomes were determined based on clinical and radiographic criteria by calibrated examiners. RESULTS: The success rates were 98.4% (63/64), 93.2% (41/44), and 89.7% (26/29) at the 6-month, 12-month, and 24-month follow-up. By the end of this study, the median follow-up period was 15.1 months, and the estimated survival rate was 95.2% at 24 months. Gender, root maturity, and number of missing walls had no significant effect on success rates. Six molars were failed, and root canal therapy (RCT) was applied. CONCLUSIONS: Partial pulpotomy for permanent molars with IP in young patients using iRoot BP Plus as pulp capping material achieved high success. This method presents a viable alternative to apexification and RCT for treating vital, inflamed molars with IP in children.

[Application of bioactive ceramics iRoot BP Plus® in pulpotomy for complicated crown fracture of immature permanent anterior teeth in children].

OBJECTIVE: To analyze the clinical and radiographic effectiveness of a calcium silicate-based bioactive ceramic iRoot BP Plus® pulpotomy of immature permanent teeth with complicated crown fracture and to evaluate the factors influencing its long-term success rate. METHODS: The digital medical records of patients under 13 years old who had undergone iRoot BP Plus® pulpotomy in the Department of Oral Emergency or the First Clinical Division, Peking University School and Hospital of Stomatology from March 2017 to September 2022 due to complicated crown fracture of anterior teeth, and had taken at least one post-operation apical radiograph were reviewed. The clinical and radiographic information at the initial examination and follow-up period were obtained, including crown color, mobility, percussion, cold test (partial pulpotomy teeth), dental restoration, fistula, swelling or inflammation of the gingival tissue, the formation of apical foramen, pathologic radiolucency and calcification of pulp chamber or root canal obliteration. Data were tested by Fisher exact test and a multiple comparison. RESULTS: In the study, 64 patients including 37 males (57.8%) and 27 females (42.2%) with a mean age of 9.1 years : ere finally enrolled. The total number of permanent teeth that received pulpotomy was 75, and the average follow-up time was 19.3 months. The success rate was 93.1% with the time interval between dental injury and treatment in 24 h, while the success rate dropped to 88.2% with the time intervals beyond 24 h. The time intervals did not significantly affect the pulp survival rate (P=0.61) after pulpotomy (partial or coronal). The success rate 6 months after pulpotomy was 96. 0%, and one-year success rate was 94. 7%. A total of 23 cases were reviewed for more than 2 years after pulpotomy, and 6 cases failed. The mobility had no significant effect on the success rate (P=0.28). Pulp chamber calcification and pulp canal obli-teration were not observed in all the post-operative radiographs. CONCLUSION: The one year clinical and radiographic success rates obtained in this study indicate that iRoot BP Plus® is an appropriate pulp capping material option for pulpotomy treatment of complicated crown fracture in immature permanent teeth without displacement injuries. This technique has broad promotional value.

Digital workflow for proximal adjustment of teeth adjacent to implant-supported fixed restorations using a predesigned computer-aided grinding guide.

Clinically, the proximal surfaces of teeth adjacent to an implant restoration usually need to be adjusted to build a preferable adjacency relationship. However, it is difficult for freehand preparation to get a favorable proximal contour in some cases. In the workflow presented here, virtual grinding can be made to adjacent teeth, under the consideration of functional reconstruction and biological requirements, and then the grinding can be implemented using digital templates and a specialized bur. This allows for more precise and accurate adjustments to be made during the clinical procedure, reducing the risk of over- or under-preparation of the proximal surfaces. In addition, the use of specialized diamond burs and grinding guides can make the procedure more efficient and streamlined, reducing the time required for proximal adjustment and minimizing patient discomfort. The resulting implant-supported prosthesis is more likely to function properly and last longer, as the precise proximal contacts can help distribute occlusal forces more evenly across the dentition. Overall, the use of digital technology for precise adjustment of proximal contacts during implant restorations represents an important advancement in modern dentistry, enabling dentists to provide their patients with more accurate, efficient, and effective dental care.

Modular Design of Highly Stable Semiconducting Porous Coordination Polymer for Efficient Electrosynthesis of Ammonia.

Developing highly stable porous coordination polymers (PCPs) with integrated electrical conductivity is crucial for advancing our understanding of electrocatalytic mechanisms and the structure-activity relationship of electrocatalysts. However, achieving this goal remains a formidable challenge because of the electrochemical instability observed in most PCPs. Herein, we develop a "modular design" strategy to construct electrochemically stable semiconducting PCP, namely, Fe-pyNDI, which incorporates a chain-type Fe-pyrazole metal cluster and π-stacking column with effective synergistic effects. The three-dimensional electron diffraction (3D ED) technique resolves the precise structure. Both theoretical and experimental investigation confirms that the π-stacking column in Fe-pyNDI can provide an efficient electron transport path and enhance the structural stability of the material. As a result, Fe-pyNDI can serve as an efficient model electrocatalyst for nitrate reduction reaction (NO3RR) to ammonia with a superior ammonia yield of 339.2 µmol h-1 cm-2 (14677 µg h-1 mgcat. -1) and a faradaic efficiency of 87 % at neutral electrolyte, which is comparable to state-of-the-art electrocatalysts. The in-situ X-ray absorption spectroscopy (XAS) reveals that during the reaction, the structure of Fe-pyNDI can be kept, while part of the Fe3+ in Fe-pyNDI was reduced in situ to Fe2+, which serves as the potential active species for NO3RR.

Conjugated Nonplanar Copper-Catecholate Conductive Metal-Organic Frameworks via Contorted Hexabenzocoronene Ligands for Electrical Conduction.

Conductive metal-organic frameworks (c-MOFs) with outstanding electrical conductivities and high charge carrier mobilities are promising candidates for electronics and optoelectronics. However, the poor solubility of planar ligands greatly hinders the synthesis and widespread applications of c-MOFs. Nonplanar ligands with excellent solubility in organic solvents are ideal alternatives to construct c-MOFs. Herein, contorted hexabenzocoronene (c-HBC) derivatives with good solubility are adopted to synthesize c-MOFs. Three c-MOFs (c-HBC-6O-Cu, c-HBC-8O-Cu, and c-HBC-12O-Cu) with substantially different geometries and packing modes have been synthesized using three multitopic catechol-based c-HBC ligands with different symmetries and coordination numbers, respectively. With more metal coordination centers and increased charge transport pathways, c-HBC-12O-Cu exhibits the highest intrinsic electrical conductivity of 3.31 S m-1. Time-resolved terahertz spectroscopy reveals high charge carrier mobilities in c-HBC-based c-MOFs, ranging from 38 to 64 cm2 V-1 s-1. This work provides a systematic and modular approach to fine-tune the structure and enrich the c-MOF family with excellent charge transport properties using nonplanar and highly soluble ligands.

Intrinsic Strain-Mediated Ultrathin Ceria Nanoantioxidant.

Metal oxide nanozymes have emerged as the most efficient and promising candidates to mimic antioxidant enzymes for treatment of oxidative stress-mediated pathophysiological disorders, but the current effectiveness is unsatisfactory due to insufficient catalytic performance. Here, we report for the first time an intrinsic strain-mediated ultrathin ceria nanoantioxidant. Surface strain in ceria with variable thicknesses and coordinatively unsaturated Ce sites was investigated by theoretical calculation analysis and then was validated by preparing ∼1.2 nm ultrathin nanoplates with ∼3.0% tensile strain in plane/∼10.0% tensile strain out of plane. Compared with nanocubes, surface strain in ultrathin nanoplates could enhance the covalency of the Ce-O bond, leading to increasing superoxide dismutase (SOD)-mimetic activity by ∼2.6-fold (1533 U/mg, in close proximity to that of natural SOD) and total antioxidant activity by ∼2.5-fold. As a proof of concept, intrinsic strain-mediated ultrathin ceria nanoplates could boost antioxidation for improved ischemic stroke treatment in vivo, significantly better than edaravone, a commonly used clinical drug.

Carbon dioxide adsorption to UiO-66: theoretical analysis of binding energy and NMR properties.

UiO-66 is one of the most valuable metal-organic frameworks because of its excellent adsorption capability for gas molecules and its high stability towards water. Herein we investigated adsorption of carbon dioxide (CO2), acetone, and methanol to infinite UiO-66 using DFT calculations on an infinite system under periodic-boundary conditions and post-Hartree-Fock (SCS-MP2 and MP2.5) calculations on cluster models. Three to four molecules are adsorbed at each of four µ-OH groups bridging three Zr atoms in one unit cell (named Site I). Six molecules are adsorbed around three pillar ligands, where the molecule is loosely surrounded by three terephthalate ligands (named Site II). Also, six molecules are adsorbed around the pillar ligand in a different manner from that at Site II, where the molecule is surrounded by three terephthalate ligands (named Site III). Totally fifteen to sixteen CO2 molecules are adsorbed into one unit cell of UiO-66. The binding energy (BE) decreases in the order Site I > Site III > Site II for all three molecules studied here and in the order acetone > methanol ≫ CO2 in the three adsorption sites. At the site I, the protonic H atom of the µ-OH group interacts strongly with the negatively charged O atom of CO2, acetone and methanol, which is the origin of the largest BE value at this site. Although the DFT calculations present these decreasing orders of BE values correctly, the correction by post-Hartree-Fock calculations is not negligibly small and must be added for obtaining better BE values. We explored NMR spectra of UiO-66 with adsorbed CO2 molecules and found that the isotropic shielding constants of the 1H atom significantly differ among no CO2, one CO2 (at Sites I, II, or III), and fifteen CO2 adsorption cases (Sites I to III) but the isotropic 17O and 13C shielding constants change moderately by adsorption of fifteen CO2 molecules. Thus, 1H NMR measurement is a useful experiment for investigating CO2 adsorption.

Nano-Impact Electrochemistry Reveals Kinetics Information of Metal-Ion Battery Materials with Multiple Redox Centers.

Prussian blue (PB) has emerged as a promising cathode material in aqueous batteries. It possesses two distinct redox centers, and the potassium ions (K+ ) are unevenly distributed throughout the compound, adding complexity to the interpretation of the K+ insertion/de-insertion kinetic mechanism. Traditional ensemble-averaged measurements are limited in uncovering the precise kinetic information of the PB particles, as the results are influenced by the construction of the porous composite electrode and the redox behavior from different particles. In this study, the electrochemical processes of individual PB particles were investigated using nano-impact electrochemistry. By varying the potentials, different types of transient current signals were obtained that revealed the kinetic mechanism of each oxidation/reduction reaction in combination with theoretical simulation. Additionally, a partially contradictory conclusion between single-particle analysis and the ensemble-averaged measurement was discussed. These findings contribute to a better understanding of the electrochemical processes of cathode materials with multiple redox centers, which facilitates the development of effective strategies to optimize these materials.

Targeted Synthesis of Isomeric Naphthalene-Based 2D Kagome Covalent Organic Frameworks.

Targeted synthesis of kagome (kgm) topologic 2D covalent organic frameworks remains challenging, presumably due to the severe dependence on building units and synthetic conditions. Herein, two isomeric "two-in-one" monomers with different lengths of substituted arms based on naphthalene core (p-Naph and m-Naph) are elaborately designed and utilized for the defined synthesis of isomeric kgm Naph-COFs. The two isomeric frameworks exhibit splendid crystallinity and showcase the same chemical composition and topologic structure with, however, different pore channels. Interestingly, C60 is able to uniformly be encapsulated into the triangle channels of m-Naph-COF via in situ incorporation method, while not the isomeric p-Naph-COF, likely due to the different pore structures of the two isomeric COFs. The resulting stable C60 @m-Naph-COF composite exhibits much higher photoconductivity than the m-Naph-COF owing to charge transfer between the conjugated skeletons and C60 guests.

Integrated Soft Porosity and Electrical Properties of Conductive-on-Insulating Metal-Organic Framework Nanocrystals.

A one-stone, two-bird method to integrate the soft porosity and electrical properties of distinct metal-organic frameworks (MOFs) into a single material involves the design of conductive-on-insulating MOF (cMOF-on-iMOF) heterostructures that allow for direct electrical control. Herein, we report the synthesis of cMOF-on-iMOF heterostructures using a seeded layer-by-layer method, in which the sorptive iMOF core is combined with chemiresistive cMOF shells. The resulting cMOF-on-iMOF heterostructures exhibit enhanced selective sorption of CO2 compared to the pristine iMOF (298 K, 1 bar, S CO 2 / H 2 ${{_{{\rm CO}{_{2}}/{\rm H}{_{2}}}}}$ from 15.4 of ZIF-7 to 43.2-152.8). This enhancement is attributed to the porous interface formed by the hybridization of both frameworks at the molecular level. Furthermore, owing to the flexible structure of the iMOF core, the cMOF-on-iMOF heterostructures with semiconductive soft porous interfaces demonstrated high flexibility in sensing and electrical "shape memory" toward acetone and CO2 . This behavior was observed through the guest-induced structural changes of the iMOF core, as revealed by the operando synchrotron grazing incidence wide-angle X-ray scattering measurements.

Fine Pore-Structure Engineering by Ligand Conformational Control of Naphthalene Diimide-Based Semiconducting Porous Coordination Polymers for Efficient Chemiresistive Gas Sensing.

Exploring new porous coordination polymers (PCPs) that have tunable structure and conductivity is attractive but remains challenging. Herein, fine pore structure engineering by ligand conformation control of naphthalene diimide (NDI)-based semiconducting PCPs with π stacking-dependent conductivity tunability is achieved. The π stacking distances and ligand conformation in these isoreticular PCPs were modulated by employing metal centers with different coordination geometries. As a result, three conjugated PCPs (Co-pyNDI, Ni-pyNDI, and Zn-pyNDI) with varying pore structure and conductivity were obtained. Their crystal structures were determined by three-dimensional electron diffraction. The through-space charge transfer and tunable pore structure in these PCPs result in modulated selectivity and sensitivity in gas sensing. Zn-pyNDI can serve as a room-temperature operable chemiresistive sensor selective to acetone.

Convergence of two serotypes within the epidemic ST11 KPC-producing Klebsiella pneumoniae creates the "Perfect Storm" in a teaching hospital.

OBJECTIVES: ST11 KPC-producing Klebsiella pneumoniae (Kp) is highly prevalent in China. We investigated the inter- and intra- host transmission and evolution characteristics of ST11 KPC-producing Kp. METHODS: A retrospective study was conducted in a hospital. The clinical data and antimicrobial resistance (AMR) phenotypes were collected. Whole genome sequencing was performed. The transmission route was reconstructed by combining single nucleotide polymorphisms (SNPs) with the clinical information. Hypervirulent Kp (HvKp) was defined as the presence of some combination of peg-344, iroB, iucA, rmpA, or rmpA2. RESULTS: Fifty-eight Kp strains isolated from thirty-five patients were enrolled. The information of one isolate was missing. The mean age of the patients was 74.3 ± 18.0 years, and 18 (50.0%) were female. Fifteen patients (41.7%, 15/36) presented with poor prognosis. All the strains were identified as ST11, and 57 strains harbored blaKPC-2. Two distinguished clades were identified based on the 1,325 high quality SNPs. In clade 1, carbapenem-resistant (CR)-hvKp accounted for 48.3% of the strains (28/58), which mostly presented as KL64 subclones, whereas CR-classical Klebsiella pneumoniae (cKp) commonly possessing KL47 were clustered in Clade 2. One CR-hvKp strain might have originated from the CR-cKp strain from within-host evolution. Even worse, a prolonged transmission of CR-hvKp has led to its spread into healthcare institutes. CONCLUSION: Two endemic subclones of ST11 KPC-producing Kp, KL64-CR-hvKp and KL47-CR-cKp, were transmitted in parallel within the hospital and/or the healthcare institute, suggesting that the ongoing genomic surveillance should be enhanced.

Rapid thermal annealing process for Se thin-film solar cells.

Recently, selenium (Se) has regained interest as a possible wide-bandgap photovoltaic material for silicon-based tandem applications. However, the easy sublimation of Se below the melting point (220 °C) brings challenges for high-quality Se thin films. Herein, we design a rapid thermal annealing (RTA) method to balance the contradiction between the sublimation and crystallization of Se thin films. Through optimizing the annealing temperature, a high-quality Se thin film is obtained with a large grain size (∼1 µm) and preferred [003] orientation during the RTA process. Then, an optimized efficiency of 3.22% is achieved in a ZnO/Se heterojunction solar cell. This study provides a new guide to obtain high-quality Se thin film by RTA and the method can be extended to other materials with high saturated vapor pressure.