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Who Does the Job? How Copper Can Replace Noble Metals in Sustainable Catalysis by the Formation of Copper-Mixed Oxide Interfaces.

ABSTRACT: Following the need for an innovative catalyst and material design in catalysis, we provide a comparative approach using pure and Pd-doped LaCu _x Mn_1-x O₃ (x = 0.3 and 0.5) perovskite catalysts to elucidate the beneficial role of the Cu/perovskite and the promoting effect of Cu _y Pd _x /perovskite interfaces developing in situ under model NO + CO reaction conditions. The observed bifunctional synergism in terms of activity and N₂ selectivity is essentially attributed to an oxygen-deficient perovskite interface, which provides efficient NO activation sites in contact with in situ exsolved surface-bound monometallic Cu and bimetallic CuPd nanoparticles. The latter promotes the decomposition of the intermediate N₂O at low temperatures, enhancing the selectivity toward N₂. We show that the intelligent Cu/perovskite interfacial design is the prerequisite to effectively replace noble metals by catalytically equally potent metal-mixed-oxide interfaces. We have provided the proof of principle for the NO + CO test reaction but anticipate the extension to a universal concept applicable to similar materials and reactions.

SUBMITTER: Thurner CW

PROVIDER: S-EPMC9251726 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Biphasic catalysis using amphiphilic polyphenols-chelated noble metals as highly active and selective catalysts.

Project description:In the field of catalysis, it is highly desired to develop novel catalysts that combine the advantages of both homogeneous and heterogeneous catalysts. Here we disclose that the use of plant polyphenol as amphiphilic large molecule ligand/stabilizer allows for the preparation of noble metal complex and noble metal nanoparticle catalysts. These catalysts are found to be highly selective and active in aqueous-organic biphasic catalysis of cinnamaldehyde and quinoline, and can be reused at least 3 times without significant loss of activity. Moreover, the catalytic activity and reusability of the catalysts can be rationally controlled by simply adjusting the content of polyphenols in the catalysts. Our strategy may be extended to design a wide range of aqueous-organic biphasic catalysis system.

| S-EPMC3714648 | biostudies-literature

Hybrid Noble-Metals/Metal-Oxide Bifunctional Nano-Heterostructure Displaying Outperforming Gas-Sensing and Photochromic Performances.

Project description:As nanomaterials are dominating 21st century's scene, multiple functionality in a single (nano)structure is becoming very appealing. Inspired by the Land of the Rising Sun, we designed a bifunctional (gas-sensor/photochromic) nanomaterial, made with TiO2 whose surface was simultaneously decorated with copper and silver (the Cu/Ag molar ratio being 3:1). This nanomaterial outperformed previous state-of-the-art TiO2-based sensors for the detection of acetone, as well as the Cu-TiO2-based photochromic material. It indeed possessed splendid sensitivity toward acetone (detection limit of 100 ppb, 5 times lower than previous state-of-the-art TiO2-based acetone sensors), as well as reduced response/recovery times at very low working temperature, 150 °C, for acetone sensing. Still, the same material showed itself to be able to (reversibly) change in color when stimulated by both UV-A and, most remarkably, visible light. Indeed, the visible-light photochromic performance was almost 3 times faster compared to the standard Cu-TiO2 photochromic material-that is, 4.0 min versus 10.8 min, respectively. It was eventually proposed that the photochromic behavior was triggered by different mechanisms, depending on the light source used.

| S-EPMC6644435 | biostudies-literature

The Role of Rare Earth Lanthanum Oxide in Polymeric Matrix Brake Composites to Replace Copper.

Project description:The main focus of current research in polymeric matrix brake composites is on searching out a replacement for copper, which has been recently proved to be a hazard to human health and the environment. In this paper, rare earth lanthanum oxide was explored for the replacement of copper in composites. The mechanism of the role of lanthanum oxide in brake composites to replace copper was analyzed. Four series of polymeric matrix brake composites with various amounts of copper (15, 10, 5 and 0 wt %) and rare earth lanthanum oxide (0, 5, 10 and 15 wt %) were developed, in which the copper was gradually replaced by lanthanum oxide in the formula. These series were characterized in terms of physical, thermo-physical and mechanical properties. The results show that lanthanum oxide can be successfully used as a replacement for copper in brake composites. Brake composites with 15 wt % lanthanum oxide that are copper-free are considered optimal, where tribo-properties are considered best. Compared with the addition of copper in brake composites, lanthanum oxide is more conducive to the formation of compacted friction films and transfer films, which is beneficial to the tribological properties of the brake composites. The addition of La₂O₃ to the brake composites can cause the reaction between La₂O₃ and Al₂O₃ to form LaAlO₃, and the reaction between Al₂O₃ and BaSO₄ can produce Ba18Al12O36 and Al₂SO₄ during the friction and wear processes, which can effectively improve the tribological properties of the brake composites at elevated temperature. This research was contributive to the copper-free, metal-free and eco-friendly brake composites.

| S-EPMC6403813 | biostudies-literature

Rapid Dissolution of Noble Metals in Organic Solvents.

Project description:The dissolution of elemental noble metals (NMs) such as gold, platinum, palladium, and copper is necessary for their recycling but carries a high environmental burden due to the use of strong acids and toxic reagents. Herein, a new approach was developed for the rapid dissolution of elemental NMs in organic solvents using mixtures of triphenylphosphine dichloride or oxalyl chloride and hydrogen peroxide, forming metal chloride salts directly. Almost quantitative dissolution of metallic Au, Pd, and Cu was observed within minutes at room temperature. For Pt, dissolution was achieved, albeit more slowly, using the chlorinating oxidant alone but was inhibited on addition of hydrogen peroxide. After leaching, transfer of PtIV and PdII chloride salts from the organic phase into a 6 m HCl aqueous phase facilitated their separation by precipitation of PtIV using a simple diamide ligand. In contrast, the retention of AuIII chloridometalate in the organic phase allowed its selective separation from Ni and Cu from a leachate solution obtained from electronic CPUs. This new approach has potential application in the hydrometallurgical leaching and purification of NMs from ores, spent catalysts, and electronic and nano-wastes.

| S-EPMC9804267 | biostudies-literature

Subsurface Carbon: A General Feature of Noble Metals.

Project description:Carbon moieties on late transition metals are regarded as poisoning agents in heterogeneous catalysis. Recent studies show the promoting catalytic role of subsurface C atoms in Pd surfaces and their existence in Ni and Pt surfaces. Here energetic and kinetic evidence obtained by accurate simulations on surface and nanoparticle models shows that such subsurface C species are a general issue to consider even in coinage noble-metal systems. Subsurface C is the most stable situation in densely packed (111) surfaces of Cu and Ag, with sinking barriers low enough to be overcome at catalytic working temperatures. Low-coordinated sites at nanoparticle edges and corners further stabilize them, even in Au, with negligible subsurface sinking barriers. The malleability of low-coordinated sites is key in the subsurface C accommodation. The incorporation of C species decreases the electron density of the surrounding metal atoms, thus affecting their chemical and catalytic activity.

| S-EPMC6471089 | biostudies-other

Controlled-Atmosphere Flame Fusion Single-Crystal Growth of Non-Noble fcc, hcp, and bcc Metals Using Copper, Cobalt, and Iron.

Project description:The growth of noble-metal single crystals via the flame fusion method was developed in the 1980s. Since then, there have been no major advancements to the technique until the recent development of the controlled-atmosphere flame fusion (CAFF) method to grow non-noble Ni single crystals. Herein, we demonstrate the generality of this method with the first preparation of fcc Cu as well as the first hcp and bcc single crystals of Co and Fe, respectively. The high quality of the single crystals was verified using scanning electron microscopy and Laue X-ray backscattering. Based on Wulff constructions, the equilibrium shapes of the single-crystal particles were studied, confirming the symmetry of the fcc, hcp, and bcc single-crystal lattices. The low cost of the CAFF method makes all kinds of high-quality non-noble single crystals independent of their lattice accessible for use in electrocatalysis, electrochemistry, surface science, and materials science.

| S-EPMC7496678 | biostudies-literature

Finding Key Factors for Efficient Water and Methanol Activation at Metals, Oxides, MXenes, and Metal/Oxide Interfaces.

Project description:Activating water and methanol is crucial in numerous catalytic, electrocatalytic, and photocatalytic reactions. Despite extensive research, the optimal active sites for water/methanol activation are yet to be unequivocally elucidated. Here, we combine transition-state searches and electronic charge analyses on various structurally different materials to identify two features of favorable O-H bond cleavage in H2O, CH3OH, and hydroxyl: (1) low barriers appear when the charge of H moieties remains approximately constant during the dissociation process, as observed on metal oxides, MXenes, and metal/oxide interfaces. Such favorable kinetics is closely related to adsorbate/substrate hydrogen bonding and is enhanced by nearly linear O-H-O angles and short O-H distances. (2) Fast dissociation is observed when the rotation of O-H bonds is facile, which is favored by weak adsorbate binding and effective orbital overlap. Interestingly, we find that the two features are energetically proportional. Finally, we find conspicuous differences between H2O/CH3OH and OH activation, which hints toward the use of carefully engineered interfaces.

| S-EPMC8788388 | biostudies-literature

Hydrogen Gas Sensing Properties of Mixed Copper-Titanium Oxide Thin Films.

Project description:Hydrogen is an efficient source of clean and environmentally friendly energy. However, because it is explosive at concentrations higher than 4%, safety issues are a great concern. As its applications are extended, the need for the production of reliable monitoring systems is urgent. In this work, mixed copper-titanium oxide ((CuTi)Ox) thin films with various copper concentrations (0-100 at.%), deposited by magnetron sputtering and annealed at 473 K, were investigated as a prospective hydrogen gas sensing material. Scanning electron microscopy was applied to determine the morphology of the thin films. Their structure and chemical composition were investigated by X-ray diffraction and X-ray photoelectron spectroscopy, respectively. The prepared films were nanocrystalline mixtures of metallic copper, cuprous oxide, and titanium anatase in the bulk, whereas at the surface only cupric oxide was found. In comparison to the literature, the (CuTi)Ox thin films already showed a sensor response to hydrogen at a relatively low operating temperature of 473 K without using any extra catalyst. The best sensor response and sensitivity to hydrogen gas were found in the mixed copper-titanium oxides containing similar atomic concentrations of both metals, i.e., 41/59 and 56/44 of Cu/Ti. Most probably, this effect is related to their similar morphology and to the simultaneous presence of Cu and Cu2O crystals in these mixed oxide films. In particular, the studies of surface oxidation state revealed that it was the same for all annealed films and consisted only of CuO. However, in view of their crystalline structure, they consisted of Cu and Cu2O nanocrystals in the thin film volume.

| S-EPMC10144612 | biostudies-literature

Machine Learning in Computational Surface Science and Catalysis: Case Studies on Water and Metal-Oxide Interfaces.

Project description:The goal of many computational physicists and chemists is the ability to bridge the gap between atomistic length scales of about a few multiples of an Ångström (Å), i. e., 10-10 m, and meso- or macroscopic length scales by virtue of simulations. The same applies to timescales. Machine learning techniques appear to bring this goal into reach. This work applies the recently published on-the-fly machine-learned force field techniques using a variant of the Gaussian approximation potentials combined with Bayesian regression and molecular dynamics as efficiently implemented in the Vienna ab initio simulation package, VASP. The generation of these force fields follows active-learning schemes. We apply these force fields to simple oxides such as MgO and more complex reducible oxides such as iron oxide, examine their generalizability, and further increase complexity by studying water adsorption on these metal oxide surfaces. We successfully examined surface properties of pristine and reconstructed MgO and Fe3O4 surfaces. However, the accurate description of water-oxide interfaces by machine-learned force fields, especially for iron oxides, remains a field offering plenty of research opportunities.

| S-EPMC7793815 | biostudies-literature

Direct functionalization of (un)protected tetrahydroisoquinoline and isochroman under iron and copper catalysis: two metals, two mechanisms.

Project description:A highly facile, straightforward synthesis of 1-(3-indolyl)-tetrahydroisoquinolines was developed using either simple copper or iron catalysts. N-protected and unprotected tetrahydroisoquinolines (THIQ) could be used as starting materials. Extension of the substrate scope of the pronucleophile from indoles to pyrroles and electron-rich arenes was realized. Additionally, methoxyphenylation is not limited to THIQ but can be carried out on isochroman as well, again employing iron and copper catalysis.

| S-EPMC3226323 | biostudies-literature

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