Direct functionalization of methane selectively to value-added chemicals is still one the main challenges in modern science. Acetic acid an important industrial chemical produced nowadays by expensive and environmentally unfriendly carbonylation methanol using homogeneous catalysts. Here, we report a new photocatalytic reaction route synthesize acetic from CH4 CO at room temperature water as sole external oxygen source. The optimized photocatalyst consists TiO2 support ammonium...

Water is essential to attain good performance in a hydrogenation reaction with ruthenium catalyst.

Iron-doped, nickel oxyhydroxide (Ni(Fe)OOH) is one of the best catalysts for oxygen evolution reaction (OER) under alkaline conditions. Due to Ni(Fe)OOH's layered structure, electrolyte species are able easily intercalate between octahedrally coordinated sheets. Electrolyte cations have long been considered inert spectator ions during electrocatalysis, but electrolytes that penetrate into catalyst may play a major role in process. In joint theoretical and experimental study, we report...

Dry reforming of methane (DRM) is an important reaction in the actual environmental and energy crisis context. It enables production syngas from CO2 CH4 reforming. While Ni catalyst presents a high activity regarding this process, it often suffers deactivation. was found that Sn-doped can avoid carbon deposition, but decrease DRM reactivity also observed. In work, we used density functional theory calculations combination with microkinetic modeling first to understand how Sn doping affects...

Carbon supported nanoparticles of monometallic Ni catalyst and binary Ni-Transition Metal (Ni-TM/C) electrocatalytic composites were synthesized via the chemical reduction method, where TM stands for doping elements Fe, Co, Cu. The composition, structure morphology Ni-TM/C materials characterized by X-ray photoelectron spectroscopy (XPS), diffraction (XRD), transmission electron microscopy (TEM), scanning (STEM) energy-dispersive (EDS). electrochemical properties towards hydrogen oxidation...

NiOOH has recently been used to catalyze water oxidation by way of electrochemical splitting. Few experimental data are available rationalize the successful catalytic capability NiOOH. Thus, theory a distinctive role for studying its properties. However, unique layered structure is associated with presence essential dispersion forces within lattice. Hence, choice an appropriate exchange-correlation functional Density Functional Theory (DFT) not straightforward. In this work, we will show...

To screen heterogeneous catalysts in silico, the linear energy relationships derived from Brønsted–Evans–Polanyi principle are extremely useful. They connect reaction of a given elementary step to its activation energy, hence providing data that can be fed kinetics models at minimal cost. However, ensure reasonable predictions, it is essential control statistical error intrinsic this approach. We several types relations for series CH and OH bond scissions simple alcohol molecules on compact...

Molecules extracted from biomass can be complex, and computing their reactivity on a catalyst is real challenge for theoretical chemistry. We present herein method to predict polyalcohol in heterogeneous catalysis. start set of simple alcohol molecules, we show that an accurate linear energy relationship constructed DFT calculations the O–H C–H dehydrogenation reactions. then this relation used fast prediction glycerol. Compared with pure calculations, our provides results good accuracy...

Considerable attention has been paid to the development of new catalysts for methanol synthesis from CO2 hydrogenation a long period time. The PdIn intermetallic catalyst was found recently exhibit good stability and activity formation. We thus performed theoretical study understand reaction mechanism on stepped PdIn(310), combining density functional theory (DFT) calculations microkinetic analysis. On basis energetics obtained clean we that preferred pathway CH3OH generation proceeds...

Abstract Solar water splitting is a promising technology to store energy in chemicals but the suffers from lack of efficient catalysts. Nickel oxyhydroxide (NiOOH) an outstanding catalyst for oxygen evolution reaction (OER). NiOOH composed partially hydrogenated nickel oxide (NiO 2 ) two‐dimensional (2D) sheets that are stacked together. Owing recent advancements fabrication it possible isolate single layer material. Such 2D catalytic systems extremely promising, especially due wider exposed...

Polyols may be associated to a large catalytic reaction network. Brønsted–Evans–Polanyi (B.E.P.) relationships aim easily predict activation barriers from energies. Acting as filter, such methods enable quickly screen all the potential intermediates and products.

The conversion of methane to valuable products is one the main challenges modern chemistry. Acetic acid (AcOH) a key chemical reagent in industry, produced nowadays by carbonylation methanol over homogeneous Rh and Ir catalysts. Here, we propose stepwise looping approach for highly selective stoichiometric synthesis AcOH with CO using single-site Pt isolated phosphotungstic anions on titania support (Pt-HPW-TiO2). reaction proceeds activation, which coincides reduction initially oxidized...

Nowadays, nanomaterials are central in modern technology, finding applications a huge variety of scientific fields, such as catalysis. Besides their chemical nature, morphology also appears to play key role catalytic processes. Although this effect has been extensively observed literature, no fundamental explanation provided yet. In work, taking anthraquinone hydrogenation on Pd model process, we used density functional theory (DFT) computation address the particle shape effect. Based...

Abstract Photoelectrochemical cells aim at producing clean fuels with solar energy. However, the major limitation of this technology is efficiency oxygen evolution reaction (OER) occurring anode electrode. One best catalysts for nickel oxyhydroxide (NiOOH) when doped iron. In work, we use Density Functional Theory (DFT)+U calculations to systematically scan various metallic dopants NiOOH. We predict that doping middle and late transition metals significantly lowers overpotential....

Abstract The computational design of solid catalysts has become a very “hot” field during the last decades, especially with recent increase in tool performance. However, theoretical techniques are still time demanding because they require consideration many adsorption configurations reaction intermediates on surface. Herein, we propose to use metal–oxygen (M−O) bond ionicity as descriptor for photocatalytic activity one best oxygen evolution (OER). Ionicity is bulk property and thus carries...

By using the pyramidalization angle as a localized geometric descriptor for oxygen reduction reaction (ORR) activity of carbon nanotubes (CNTs), we show ORR these systems can be readily predicted with mere structural optimization CNTs.

Abstract Fischer‐Tropsch synthesis (FTS) is an attractive opportunity to prepare fuels and chemicals, avoiding fossil resources exploration. Co 2 C was recently demonstrated exhibit outstanding properties in olefins (FTO) reaction, inhibiting methane formation. However, the exact mechanisms have not been entirely revealed yet. Here we are proposing a study combining DFT calculations microkinetic modelling (MKM) order unveil dominant reaction pathways of three products interest FTS, namely...

To computationally design efficient solid catalysts, density functional theory (DFT) calculations are widely used in combination with microkinetic modeling (MKM). However, MKM results often biased due to the overestimation of adsorption strength DFT that usually performed at an arbitrary low coverage surface intermediates. We hereby developed a new iterative approach focusing on main species present catalyst steady state, hence allowing energy calculation only presence relevant In this way,...

Within conventional bifunctional catalysts, active metal sites are associated with components, while acid usually localized over oxide supports. The modification of by halogens provides an opportunity to generate acidity via the heterolytic dissociation hydrogen directly sites. Herein, we report results high-throughput screening combinations different metals (Co, Ni, Ru, Pt, Pd, Rh) and (Cl, Br, I) for site generation from in hydrogenation furfural 5-hydroxymethylfurfural. demonstrate that...