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A core–shell structured Mg(OH)2/PS with enhanced surface lipophilicity was successfully synthesized by a microemulsion template. The core magnesium hydroxide was prepared in a cetyltrimethyl ammonium bromide (CTAB)/isopropanol/cyclohexane/water microemulsion, and the shell polystyrene (PS) was formed in situ by adding styrene monomer into oil phase of the microemulsion. The Mg(OH)2/PS core–shell nanoparticles were characterized by X‐ray diffraction (XRD), scanning electron microscopy (SEM), X‐ray photoelectron spectroscopy (XPS), thermogravimetry/differential scanning calorimetry (TG/DSC) and Fourier transform infrared spectroscopy (FT‐IR). The results indicated that the obtained nanoparticles is a core–shell structure and well‐dispersed; the polystyrene shell thicknesses could be controlled in the range of 9.11 to 13.36 nm by simply changing the dosage of styrene monomer. Due to its polymer coating modification and integrated core–shell structure, the Mg(OH)2/PS is with excellent surface lipophilicity and easy to mix with the organic phase. The results provide a facile method to produce the surface‐modified inorganic material for functionality.

Selective hydrogenation of aromatic amines, especially chemicals such as aniline and bis(4-aminocyclohexyl)methane for non-yellowing polyurethane, is of particular interests due to the extensive applications. To conquer the existing difficulties in selective hydrogenation, the Ru0-Ruδ+/CeO2 catalyst with solid frustrated Lewis pairs was developed for aromatic amines hydrogenation with excellent activity and selectivity under relative milder conditions. The morphology, electronic and chemical properties, especially the Ru0-Ruδ+ clusters and reducible ceria were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electronic microscopy (SEM), X-ray photoelectron spectroscopy (XPS), CO2 temperature programmed desorption (CO2-TPD), H2 temperature programmed reduction (H2-TPR), H2 diffuse reflectance Fourier transform infrared spectroscopy (H2-DRIFT), Raman, etc. The 2% Ru/CeO2 catalyst exhibited good conversion of 95% and selectivity greater than 99% toward cyclohexylamine. The volcano curve describing the activity and Ru state was found. Owning to the "acidic site isolation" by surrounding alkaline sites, condensation between the neighboring amine molecules could be effectively suppressed. The catalyst also showed good stability and applicability for other aromatic amines and heteroarenes containing different functional groups.

The transformation of levulinic acid (LA) into γ-valerolactone (GVL) in water at room temperature is very interesting. In this work, we designed and prepared single Ru atoms on a TiO2@nitrogen doped porous carbon support catalyst (Ru/TiO2@CN). It was demonstrated that the catalyst had very high activity, selectivity and stability for the conversion of LA into GVL at room temperature in water. The turnover frequency (TOF) could reach 278 molGVL molRu−1 h−1 at complete conversion, which was about 35 times higher than that of commercial Ru/C. In addition, only GVL was generated in the reaction over the catalyst of this work.

This work describes the highly efficient Pd-catalyzed direct coupling of aryl ethers (including the typical lignin model compounds) and morpholines to produce 4-cyclohexylmorpholines, a useful class of fine chemicals. Without employing any acidic additives, various 4-cyclohexylmorpholines could be synthesized with good yields from a variety of aryl ethers using H2 as a hydrogen resource. A mechanism study revealed that the desired product was formed via the cleavage of the C(Ar)–O bonds to generate the corresponding cyclohexanones and subsequent reductive amination.

Partially removing the framework Al atoms from low-silica aluminosilicates is an old but still challenging problem, because a high framework Al content generally induces lower acid strength and fast deactivation. An inappropriate dealumination method may cause structural collapse. The organic structure-directing agent (OSDA)-free Beta zeolite is expected to serve as a green solid acid catalyst, but decreasing the Al content before being used as a catalyst is needed to enhance the stability and acid strength. Al2(SO4)3 was used to extract effectively the framework Al species from Al-rich OSDA-free Beta (Si/Al = 4.3) under mild conditions, forming a natroalunite phase. The natroalunite phase was then selectively washed away with diluted NaOH solution, resulting in dealuminated zeolite (DeAl Beta) with a pure *BEA phase and higher Si/Al ratios of 7.6–12. The dealuminated Beta zeolites were revealed to possess abundant mesopores while maintaining high crystallinity. The decrease of the total acid amount in DeAl Beta zeolites was accompanied by the enhancement of acid strength, resulting in higher selectivity of deeper cracking products and lower deactivation rate in the 1,3,5-triisopropylbenzene cracking reaction. The DeAl Beta also showed a high catalytic activity comparable to commercial nanosized Beta in the liquid-phase Friedel–Crafts acylation, which was much higher than the parent Al-rich Beta. This study would provide a promising method for developing useful solid acid catalysts by the combination of OSDA-free synthesis and the eco-efficient dealumination process.

The transformation of renewable lignin-based platform chemicals into value-added nitrogen-containing compounds is an emerging strategy for lignin utilization. However, multi-reactive sites on these platform chemicals make it challenging to control the product selectivity, thereby resulting in limited success. In this work, we developed the reductive-coupling of guaiacol, a typical lignin-based platform chemical, with amines and H2 to synthesize methoxy-functionalized cyclohexylamines. It was demonstrated that Pd/C was a very efficient catalyst for this kind of reaction, and high yields of the target products can be obtained. Notably, this methodology can be applied for the reductive-coupling of various guaiacol analogues with amines to synthesize alkoxyl-functionalized cyclohexylamines with high yields. A mechanism study revealed that the reaction occurred through the generation of 2-methoxycyclohexanone and its subsequent reductive amination.

Methanol-to-olefins (MTO) technology presently serves as a key to convert coal or natural gas to valuable hydrocarbons, in particular lower olefins. This work focuses on developing a low cost and environmentally benign MTO catalyst from low-silica CHA zeolite. Its moderate acidity and reaction space have been balanced by tuning the residual K+ cations in the cavity via controlled ammonium ion-exchange. The structure-dependent catalytic performances have been assessed, summarized and discussed by using various characterization techniques. The crystalline structure and crystal morphology of CHA were well preserved during the NH4+ exchange. N2 physisorption demonstrated that the pore volume and specific surface area increased substantially after K+ cations were exchanged as a result of pore opening. NH3 temperature-programmed desorption (TPD) and NH3-adsorption IR spectra showed that the amount and strength of acid sites were regulated by the exchange level of K+ with NH4+, which was closely related to the K+ location according to NO and acetonitrile adsorption IR spectra. The completely exchanged CHA (>98% K+ exchange level) deactivated rapidly in MTO at 400 °C, whereas CHA (65% K+ exchange level) with moderate acidity showed the best catalytic performance. The moderate acidity in the open cage facilitated the formation of higher methylbenzene intermediates, giving propylene (45%) as the predominant product.

Background: The Platelet Inhibition and Patient Outcomes (PLATO) study found that ticagrelor plus aspirin (TA) was more effective than clopidogrel plus aspirin (CA), without an increase in the risk of massive bleeding in patients undergoing percutaneous coronary intervention (PCI). Data from other studies indicate that the conclusion is controversial with the results obtained by PLATO. Aim: To investigate the efficacy and safety of TA, compared with CA, in patients with acute coronary syndrome (ACS) after PCI. Methods: A systematic literature search was performed in the MEDLINE, EMBASE, and Cochrane databases to compare the efficacy and safety of CA and TA treatment in patients with ACS after PCI. The endpoints were major adverse cardiac events (MACEs), death, stroke, myocardial infarction (MI), stent thrombosis, and bleeding events. The data analysis was performed using RevMan 5.3 software, and the odds ratios (ORs) and their 95% confidence intervals (CI) were calculated. The standards of reporting were in accordance with the PRISMA guidelines. Results: 13 studies with a total of 58,062 patients were included in this study with a subgroup analysis of the European/American and Asian populations. In terms of effectiveness for MACEs, the European, American and Asian populations benefitted more from the TA treatment than the CA treatment (European and American populations, OR = 0.82, P = 0.0002; Asian, OR = 0.66, P Conclusion: The TA treatment in the European and American populations is more beneficial and safer than CA treatment. However, although the Asian population has this benefit, the risk of bleeding is significantly increased as well, and antiplatelet drugs should be chosen carefully.

The first example of highly enantioselective fluoroarylation of gem -difluoroalkenes with aryl halides is presented by using a new chiral sulfinamide phosphine ( Sadphos ) type ligand TY-Phos . N -Me- TY-Phos can be easily synthesized on a gram scale from readily available starting materials in 3 steps. Salient features of this work including readily available starting materials, good yields, high enantioselectivities as well as broad substrate scope make this approach very practical and attractive. Notably, the asymmetric synthesis of an analogue of a biologically active molecule is also reported.

We report a facile and economical synthesis of α-fluoroacrylic acids via direct electrochemical defluorinative carboxylation of gem-difluoroalkenes with CO2. By using a platinum plate as the working cathode and a cheap nickel plate as the anode in a user-friendly undivided cell under constant current conditions, the reactions proceed smoothly under room temperature, without the use of expensive transition metal catalysts, ligands, external base or reductant, affording the desired adducts in up to 83% yield and 20:1 Z/E ratio, with good functional group tolerance. A cyclic voltammetry study was conducted and suggested a novel ECEC process.

Electrochemical CO2 reduction is of great importance for both decreasing greenhouse gas concentration and producing value-added chemicals and fuels. CO is the key industrial feedstock for the synth...

The exploration of efficient electrocatalysts for the reduction of CO2 to C2H4 is of significant importance but is also a challenging subject. Cu-based bimetallic catalysts are extremely promising for efficient CO2 reduction. In this work, we synthesize a series of porous bimetallic Cu–Sb alloys with different compositions for the catalytic reduction of CO2 to C2H4. It is demonstrated that the alloy catalysts are much more efficient than the pure Cu catalyst. The performance of the alloy catalysts depended strongly on the composition. Further, the alloy with a Cu:Sb ratio of 10:1 yielded the best results; it exhibited a high C2H4 Faradaic efficiency of 49.7% and a high current density of 28.5 mA cm−2 at −1.19 V vs. a reversible hydrogen electrode (RHE) in 0.1 M KCl solution. To the best of our knowledge, the electrocatalytic reduction of CO2 to C2H4 using Cu–Sb alloys as catalysts has not been reported. The excellent performance of the porous alloy catalyst is attributed to its favorable electronic configuration, large surface area, high CO2 adsorption rate, and fast charge transfer rate.

Electrocatalytic reduction of CO2 to a single product at high current densities and efficiencies remains a challenge. However, the conventional electrode preparation methods, such as drop-casting, usually suffer from low intrinsic activity. Herein, we report a synthesis strategy for preparing heterogeneous electrocatalyst composed of 3D hierarchical Cu dendrites that derived from an in situ electrosynthesized hollow copper metal-organic framework (MOF), for which the preparation of the Cu-MOF film took only 5 min. The synthesis strategy preferentially exposes active sites, which favor's the reduction of CO2 to formate. The current density could be as high as 102.1 mA cm-2 with a selectivity of 98.2 % in ionic-liquid-based electrolyte and a commonly used H-type cell.

An enantioselective carboxylative cyclization of propargylic alcohols and CO2 was realized under mild conditions, based on a kinetic resolution strategy, which enabled the synthesis of chiral cyclic carbonates and propargylic alcohols with promising yield and enantioselectivity simultaneously.

Objective: We aimed to explore the safety and diagnostic value of medical thoracoscopic lung biopsy in patients with unexplained diffuse interstitial lung disease (ILD) in a single center pilot study. Method: We retrospectively analyzed clinical and pathological diagnostic data from 52 patients with diffuse ILD undergoing medical thoracoscopic lung biopsy. Results: Forty-four cases of diffuse ILD were confirmed pathologically, giving a diagnostic rate of 84.6%. Among these 44 patients, 11 patients were diagnosed with cancer, including 8 patients with lung adenocarcinoma, 3 patients with metastases; 2 from a gastrointestinal malignancy, and 1 from a granulosa cell tumor of the ovary. There were 17 cases of idiopathic interstitial pneumonia, including 9 cases of usual interstitial pneumonia (UIP), 4 cases of non-specific interstitial pneumonia (NSIP), 3 cases of cryptogenic organizing pneumonia (COP), and 1 case of acute interstitial pneumonia (AIP). There were 12 cases of rare interstitial pneumonias, which included 6 cases of pulmonary alveolar proteinosis, 1 case each of pulmonary Langerhans cell histiocytosis (LCH) and pulmonary lymphangiomyomatosis, 2 cases of nodular sarcoidosis, and 2 cases of chronic eosinophilic pneumonia. We recorded various complications, including bleeding, infection, and pneumothorax. A total of 28 patients (53.8%) experienced at least one of the above complications, but there were no deaths associated with biopsy. Conclusions: Medical thoracoscopic lung biopsy appears a safe and effective method for diagnosing diffuse ILD of unknown cause but further prospective studies, with larger numbers, including comparison with other established techniques are required.

Low-temperature and selective reductive amination of carbonyl compounds is a highly promising approach to access primary amines. However, it remains a great challenge to conduct this attractive route efficiently over earth-abundant metal-based catalysts. Herein, we designed several Co-based catalysts (denoted as Co@C-N(

Chronic obstructive pulmonary disease (COPD) is the most common chronic inflammatory airway disease. Il-12r beta 2 (We recruited 996 participants to perform an association analysis through SNPStats online software. We used false-positive report probability analysis to detect whether the positive findings were noteworthy. Haploview 4.2 software and SNPStats were used to conduct the haplotype analysis and linkage disequilibrium. Finally, the interaction of SNP-SNP in COPD risk was evaluated by multi-factor dimensionality reduction.The study found evidence that genetic loci inIntronic variants in

Use of multi-metallic catalysts to enhance reactions is an interesting research area, which has attracted much attention. In this work, we carried out the first work to prepare trimetallic electrocatalysts by a one-step co-electrodeposition process. A series of Cu-X-Y (X and Y denote different metals) catalysts were fabricated using this method. It was found that Cu

The asymmetric denitrogenative cycloaddition has emerged as a powerful tool to build chiral aza-heterocyles. However, only one example of asymmetric denitrogenative cycloaddition of benzotriazole with unsaturated hydrocarbons has been explored so far, because the ring-opening of benzotriazole to generate α-imino metal carbenoid species is a thermodynamically unfavorable process. We herein report an efficient asymmetric denitrogenative cycloaddition of benzotriazoles with cyclic and acyclic 1,3-dienes enabled by Pd and chiral sulfonamide phosphine ligand. A variety of substituted hexahydrocarbazoles and indolines were delivered in good yields with high ee values. Interestingly, a pair of enantiomers could be obtained with the use of Xu1 and PC2 with the same absolute configuration. The synthetic utilities of the optically active hexahydrocarbazoles were also showcased.

A highly enantioselective palladium/WJ-Phos-catalyzed Suzuki–Miyaura coupling reaction for efficient construction of axially chiral biaryl monophosphine oxides was developed. A series of axially ch...

Cu–Pd bimetallic catalysts were fabricated on carbon paper (CP) by the electrodeposition method via a dynamic hydrogen bubble template approach. At a potential of −1.2 V vs. RHE, the Faradaic efficiency (FE) of C2H4 could reach 45.2% with a current density of 17.4 mA cm−2 in an H-type electrolytic cell. Detailed studies suggest that the enhanced performance of Cu–Pd/CP was attributed mainly to the synergistic effect, low interfacial charge transfer resistance, and the 3D architecture of the catalysts.

A highly chemo-, regio-, enantio-selectivitive Pd/Xiang-Phos-catalyzed intermolecular carboheterofunctionalization of 2,3-dihydrofurans for the synthesis of polysubstituted benzofused heterocycles mild conditions., A mild and practical Pd/Xiang-Phos-catalyzed enantioselective intermolecular carboheterofunctionalization reaction of 2,3-dihydrofurans is developed, leading to various optically active fused furoindolines and tetrahydrofurobenzofurans. The key to this transformation is employing two newly modified N-Me-Xiang-Phos ligands ((S, RS)-N-Me-X4/X5) as chiral ligands under mild conditions. Moreover, this synthetic methodology can be efficiently applied to a variety of complex polysubstituted heterocycles with high chemo-, regio-, and enantio-selectivities via introducing diverse substituents on furan rings, which were hard to access by other routes.

Sn4P3/reduced graphene oxide nanocomposites exhibited high selectivity for CO over a wide potential range from −2.2 V to −2.5 V vs. Ag/Ag+. The maximum faradaic efficiency for CO can reach 96.6% with a high current density of 68.0 mA cm−2. The high efficiency and selectivity can be attributed to the modified electronic structure of Sn sites, the small Sn4P3 nanoparticles and their dense packing in a conductive matrix, leading to a high density of active sites for adsorbing CO2 and stabilizing the CO2˙− intermediate.

Cuprous oxide catalysts have attracted much attention because they exhibited high selectivity of C2+ products in CO2 electroreduction, but the effect of the structure of catalysts on the reaction needs to be studied further. Herein, we studied the effect of the coordination number (CN) of Cu–Cu and Cu–O in Cu2O on the catalytic performance of CO2 electrocatalytic reduction to C2H4. It was demonstrated that Cu–Cu CN and Cu–O CN, which could be tuned by changing the crystal surface and size of Cu2O, influenced the current density and faradaic efficiency (FE) of C2H4 significantly. At suitable CNs, the FE of C2H4 could reach 50.6% with a current density of 24.5 mA cm−2.

A thorough investigation of the nature of the Ti species in the boron-containing Ti-MWW zeolite has been carried out. It was found that the inactive extra-framework TiO6 species can cover up the zeolite Lewis-acid property through the weak atomic binding forces between the “Ti(IV)” atom and “O” atom (TiO6 species). The nitric acid treatment could remove these TiO6 species easily from the as-synthesized Ti-MWW(P), followed by exposure of the zeolite Lewis acidity. Importantly, the formation of new Ti(OSi)3OH species with a strong Lewis-acid strength, is facilitated in the modification process. Thereby, the modified Ti-MWW zeolite has an improved catalytic activity in alkene epoxidation reactions. The removal of framework B(IV) species around the TiO4 species is an essential step because it can accelerate the transformation of perfect Ti(OSi)4 species to the defective Ti(OSi)3OH species in zeolites. Moreover, the strategy to construct Ti(OSi)3OH species was also applied successfully in boron-containing Ti-MCM-56 zeolites. Considering active species environment can be modulated effectively with the removal of framework tetra-coordinate boron, this strategy could also be beneficial for the preparation of other high-performance titanosilicates.

Highly dispersed metallic silver nanoparticles (AgNPs) are promising heterogeneous catalysts for carboxylative coupling of terminal alkynes with CO2 under mild conditions. Yet, their size-controlled synthesis is very challenging because of the high surface energy. Here, we prepared a series of amino-functionalized ordered mesoporous polymers as hosts for anchoring AgNPs. Control experiments and computations showed that electron-rich amines were confined in mesochannels with varying electron density and steric hindrance, creating "localized active zones (LAZ)" to control the growth of AgNPs. The particle size of AgNPs grows along with the increased volume of LAZ around nitrogen species. We also revealed that the catalytic activity of Ag-based catalysts is size-dependent and increases with decreasing particle size. Building on these findings, we report a facile one-pot synthesis strategy for preparing an amine-incorporated ordered mesoporous polymer (NOMP) with a high specific surface area, small LAZ volume, and uniform amine sites with controllable loading. These features result in the formation of ultrasmall and monodispersed Ag nanoparticles. Remarkably, Ag@NOMP gave a quantitative target yield under the conditions of 1 atm CO2 pressure and 50 °C, showing superior catalytic activity in CO2 carboxylation compared to other mesoporous analogues.

Protein-based NMR spectroscopy has proven to be a very robust method for finding fragment leads to protein targets. However, one limitation of protein-based NMR is that the data acquisition and analysis can be time consuming. In order to streamline the scoring of protein-based NMR fragment screening data and the determination of ligand affinities using 2D NMR experiments we have developed a data analysis workflow based on principal component analysis (PCA) within the TREND NMR Pro software package. We illustrate this using four different proteins and sets of ligands which interact with these proteins over a range of affinities. Also, these PCA-based methods can be successfully applied even to systems where ligand binding to target proteins is in intermediate or even slow exchange on the NMR time scale. Finally, these methods will work for scoring of fragment binding data using protein spectra that are either highly overlapped or lower in resolution.

A gold-catalyzed enantioselective cyclopropanation of enamides with α-diazoarylacetate compounds was developed, which provides a facile access to synthetically useful densely substituted cyclopropanes in good yields with excellent enantioselectivities and diastereoselectivities.

The highly enantioselective copper-catalyzed three-component boroacylation of 1,1-disubstituted allenes is reported by using a class of chiral ligands (WJ-Phos), delivering various functionalized o...

We report an efficient Au(I)-catalyzed formal allylation of diazo(thio)oxindoles using allyltrimethylsilane to give 3-allyl (thio)oxindoles, which are difficult to access by using traditional alkylation methods under basic conditions. The approach enables a highly stereoselective synthesis of quaternary (thio)oxindoles via a formal allylation-asymmetric Michael addition sequence. These adducts are versatile synthons for spirocyclic (thio)oxindoles. Initial biological studies reveal that chiral thiooxindoles show promising antiproliferation activity that is better than that of the corresponding oxindoles.

A novel, simple, effective and rapid synthetic method to construct the C-2 trifluoromethylated indolinyl ketones via a copper-catalyzed cyclization reaction between N-alkylaniline and β-(trifluoromethyl)-α,β-unsaturated enones was developed. The results of the control experiments show that the reaction may involve a radical mechanism by a single-electron transfer process. Moreover, a broad substrate scope and good functional groups, high diastereoselectivities (dr, up to >20 : 1) as well as gram-scale synthesis make this approach highly attractive.

Supplemental material, sj-pdf-2-tar-10.1177_1753466620986390 for Assessment and review of treatment for secondary spontaneous pneumothorax using medical thoracoscopy-assisted argon plasma coagulation in association with autologous blood pleurodesis by Lei Zhang, Tian Xie, Yihui Fu and Haihong Wu in Therapeutic Advances in Respiratory Disease

Supplemental material, sj-pdf-4-tar-10.1177_1753466620986390 for Assessment and review of treatment for secondary spontaneous pneumothorax using medical thoracoscopy-assisted argon plasma coagulation in association with autologous blood pleurodesis by Lei Zhang, Tian Xie, Yihui Fu and Haihong Wu in Therapeutic Advances in Respiratory Disease

Supplemental material, sj-pdf-3-tar-10.1177_1753466620986390 for Assessment and review of treatment for secondary spontaneous pneumothorax using medical thoracoscopy-assisted argon plasma coagulation in association with autologous blood pleurodesis by Lei Zhang, Tian Xie, Yihui Fu and Haihong Wu in Therapeutic Advances in Respiratory Disease

Supplemental material, sj-pdf-1-tar-10.1177_1753466620986390 for Assessment and review of treatment for secondary spontaneous pneumothorax using medical thoracoscopy-assisted argon plasma coagulation in association with autologous blood pleurodesis by Lei Zhang, Tian Xie, Yihui Fu and Haihong Wu in Therapeutic Advances in Respiratory Disease

Electroreduction of CO2 to liquid fuels such as ethanol and n-propanol, powered by renewable electricity, offers a promising strategy for controlling the global carbon balance and addressing the need for the storage of intermittent renewable energy. In this work, we discovered that the composite composed of nitrogen-doped graphene quantum dots (NGQ) on CuO-derived Cu nanorods (NGQ/Cu-nr) was an outstanding electrocatalyst for the reduction of CO2 to ethanol and n-propanol. The Faradaic efficiency (FE) of C2+ alcohols could reach 52.4 % with a total current density of 282.1 mA cm-2 . This is the highest FE for C2+ alcohols with a commercial current density to date. Control experiments and DFT studies show that the NGQ/Cu-nr could provide dual catalytic active sites and could stabilize the CH2 CHO intermediate to enhance the FE of alcohols significantly through further carbon protonation. The NGQ and Cu-nr had excellent synergistic effects for accelerating the reduction of CO2 to alcohols.