Additional file 1 of Quantitative proteomics identified circulating biomarkers in lung adenocarcinoma diagnosis

Additional file 1: Table S1. Differentially expressed proteins identified in plasma samples

Choses et gens de la Martinique, ce que la Martinique demande à la France / André Delaunay-Belleville

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Atomic Resolution Imaging of Nanoscale Structural Ordering in a Complex Metal Oxide Catalyst

The determination of the atomic structure of a functional material is crucial to understanding its “structure-to-property” relationship (e.g., the active sites in a catalyst), which is however challenging if the structure possesses complex inhomogeneities. Here, we report an atomic structure study of an important MoVTeO complex metal oxide catalyst that is potentially useful for the industrially relevant propane-based BP/SOHIO process. We combined aberration-corrected scanning transmission electron microscopy with synchrotron powder X-ray crystallography to explore the structure at both nanoscopic and macroscopic scales. At the nanoscopic scale, this material exhibits structural and compositional order within nanosized “domains”, while the domains show disordered distribution at the macroscopic scale. We proposed that the intradomain compositional ordering and the interdomain electric dipolar interaction synergistically induce the displacement of Te atoms in the Mo–V–O channels, which determines the geometry of the multifunctional metal oxo-active sites

Unravelling Thiol’s Role in Directing Asymmetric Growth of Au Nanorod–Au Nanoparticle Dimers

Asymmetric nanocrystals have practical significance in nanotechnologies but present fundamental synthetic challenges. Thiol ligands have proven effective in breaking the symmetric growth of metallic nanocrystals but their exact roles in the synthesis remain elusive. Here, we synthesized an unprecedented Au nanorod–Au nanoparticle (AuNR–AuNP) dimer structure with the assistance of a thiol ligand. On the basis of our experimental observations, we unraveled for the first time that the thiol could cause an inhomogeneous distribution of surface strains on the seed crystals as well as a modulated reduction rate of metal precursors, which jointly induced the asymmetric growth of monometallic dimers

Investigating the Influence of Mesoporosity in Zeolite Beta on Its Catalytic Performance for the Conversion of Methanol to Hydrocarbons

Hierarchically porous zeolite Beta (Beta-MS) synthesized by a soft-templating method contains remarkable intracrystalline mesoporosity, which reduces the diffusion length in zeolite channels down to several nanometers and alters the distribution of Al among distinct crystallographic sites. When it was used as a catalyst for the conversion of methanol to hydrocarbons (MTH) at 330 °C, Beta-MS exhibited a 2.7-fold larger conversion capacity, a 2.0-fold faster reaction rate, and a remarkably longer lifetime in comparison to conventional zeolite beta (Beta-C). The superior catalytic performance of Beta-MS is attributed to its hierarchical structure, which offers full accessibility to all catalytically active sites. In contrast, Beta-C was easily deactivated because a layer of coke quickly deposited on the outer surfaces of the catalyst crystals, impeding access to interior active sites. This difference is clearly demonstrated by using electron microscopy combined with electron energy loss spectroscopy to probe the distribution of coke in the deactivated catalysts. At both low and high conversions, ranging from 20% to 100%, Beta-MS gave higher selectivity toward higher aliphatics (C₄–C₇) but lower ethene selectivity in comparison to Beta-C. Therefore, we conclude that a hierarchical structure decreases the residence time of methylbenzenes in zeolite micropores, disfavoring the propagation of the aromatic-based catalytic cycle. This conclusion is consistent with a recent report on ZSM-5 and is also strongly supported by our analysis of soluble coke species residing in the catalysts. Moreover, we identified an oxygen-containing compound, 4-methylbenzaldehyde, in the coke, which has not been observed in the MTH reaction before

Cu-TDPAT, an <i>rht</i>-Type Dual-Functional Metal–Organic Framework Offering Significant Potential for Use in H₂ and Natural Gas Purification Processes Operating at High Pressures

The separations of CO₂/CO/CH₄/H₂, CO₂/H₂, CH₄/H₂, and CO₂/CH₄ mixtures at pressures ranging to 7 MPa are important in a variety of contexts, including H₂ production, natural gas purification, and fuel-gas processing. The primary objective of this study is to demonstrate the selective adsorption potential of an <i>rht</i>-type metal–organic framework [Cu₃(TDPAT)­(H₂O)₃]·10H₂O·5DMA (Cu-TDPAT), possessing a high density of both open metal sites and Lewis basic sites. Experimental high pressure pure component isotherm data for CO₂, CO, CH₄, and H₂ are combined with the Ideal Adsorbed Solution Theory (IAST) for estimation of mixture adsorption equilibrium. The separation performance of Cu-TDPAT is compared with four other microporous materials, specifically chosen in order to span a wide range of physicochemical characteristics: MgMOF-74, MIL-101, LTA-5A, and NaX. For all mixtures investigated, the capacity of Cu-TDPAT to produce the desired product, H₂ or CH₄, satisfying stringent purity requirements, in a fixed bed operating at pressures exceeding about 4 MPa, is either comparable to, or exceeds, that of other materials

Synthesis and Gas Transport Properties of Hydroxyl-Functionalized Polyimides with Intrinsic Microporosity

A newly designed diamine monomer, 3,3,3′,3′-tetramethyl-1,1′-spirobisindane-5,5′-diamino-6,6′-diol, was successfully used to synthesize two types of polyimides for membrane-based gas separation applications. The novel polymers integrate significant microporosity and polar hydroxyl groups, showing the combined features of polymers of intrinsic microporosity (PIMs) and functional polyimides (PIs). They possess high thermal stability, good solubility, and easy processability for membrane fabrication; the resulting membranes exhibit good permeability owing to the intrinsic microporosity introduced by the highly contorted PIM segments as well as high CO₂/CH₄ selectivity that arises from the hydroxyl groups. The membranes show CO₂/CH₄ selectivities of >20 when tested with a 1:1 CO₂/CH₄ mixture for feed pressures up to 50 bar. In addition, the incorporation of hydroxyl groups and microporosity in the polymers enhances their affinity to water, leading to remarkable water sorption capacities of up to 22 wt % at 35 °C and 95% relative humidity

Chiral Gold Nanowires with Boerdijk–Coxeter–Bernal Structure

A Boerdijk–Coxeter–Bernal (BCB) helix is made of linearly stacked regular tetrahedra (<i>tetrahelix</i>). As such, it is chiral without nontrivial translational or rotational symmetries. We demonstrate here an example of the chiral BCB structure made of totally symmetrical gold atoms, created in nanowires by direct chemical synthesis. Detailed study by high-resolution electron microscopy illustrates their elegant chiral structure and the unique one-dimensional “pseudo-periodicity”. The BCB-type atomic packing mode is proposed to be a result of the competition and compromise between the lattice and surface energy

Strong Metal–Support Interactions Achieved by Hydroxide-to-Oxide Support Transformation for Preparation of Sinter-Resistant Gold Nanoparticle Catalysts

The strong metal–support interactions (SMSI) are well-known but crucial for preparation of supported metal nanoparticle catalysts, which generally occur by reduction and oxidation under harsh conditions. Here, we delineate the example of constructing SMSI without reduction and oxidation, where the key is to employ a hydroxide-to-oxide support transformation. The covering of Au nanoparticles by oxides, electronic interaction, and changes in CO adsorption tests of the catalyst are identical to those of the classic SMSI. Owing to the SMSI with oxide barriers on the Au nanoparticles, the supported Au catalysts are sintering-resistant at high temperatures, which benefit long-life reactions, outperforming the conventional supported catalysts

High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst

Hydrogen evolution reaction (HER) is a critical process due to its fundamental role in electrocatalysis. Practically, the development of high-performance electrocatalysts for HER in alkaline media is of great importance for the conversion of renewable energy to hydrogen fuel via photoelectrochemical water splitting. However, both mechanistic exploration and materials development for HER under alkaline conditions are very limited. Precious Pt metal, which still serves as the state-of-the-art catalyst for HER, is unable to guarantee a sustainable hydrogen supply. Here we report an anomalously structured Ru catalyst that shows 2.5 times higher hydrogen generation rate than Pt and is among the most active HER electrocatalysts yet reported in alkaline solutions. The identification of new face-centered cubic crystallographic structure of Ru nanoparticles was investigated by high-resolution transmission electron microscopy imaging, and its formation mechanism was revealed by spectroscopic characterization and theoretical analysis. For the first time, it is found that the Ru nanocatalyst showed a pronounced effect of the crystal structure on the electrocatalytic activity tested under different conditions. The combination of electrochemical reaction rate measurements and density functional theory computation shows that the high activity of anomalous Ru catalyst in alkaline solution originates from its suitable adsorption energies to some key reaction intermediates and reaction kinetics in the HER process