Browse
Submit Data
Databases
API
Help

Dataset Information

0 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

BNPd single-atom catalysts for selective hydrogenation of acetylene to ethylene: a density functional theory study.

ABSTRACT: The mechanisms of selective hydrogenation of acetylene to ethylene on B11N12Pd single-atom catalyst were investigated through the density functional theory by using the 6-31++G** basis set. We studied the adsorption characteristics of H2 and C2H2, and simulated the reaction mechanism. We discovered that H2 underwent absolute dissociative chemisorption on single-atom Pd, forming the B11N12Pd(2H) dihydride complex, and then the hydrogenation reaction with C2H2 proceeded. The hydrogenation reaction of acetylene on the B11N12Pd complex complies with the Horiuti-Polanyi mechanism, and the energy barrier was as low as 26.55?kcal?mol-1. Meanwhile, it also has a higher selectivity than many bimetallic alloy single-atom catalysts.

SUBMITTER: Gong W

PROVIDER: S-EPMC6083668 | biostudies-literature | 2018 Jul

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Publications

BNPd single-atom catalysts for selective hydrogenation of acetylene to ethylene: a density functional theory study.

Gong Wanqi W Kang Lihua L

Royal Society open science 20180725 7

The mechanisms of selective hydrogenation of acetylene to ethylene on B11N12Pd single-atom catalyst were investigated through the density functional theory by using the 6-31++G** basis set. We studied the adsorption characteristics of H2 and C2H2, and simulated the reaction mechanism. We discovered that H2 underwent absolute dissociative chemisorption on single-atom Pd, forming the B11N12Pd(2H) dihydride comp ...[more]

PMID: 30109043

Similar Datasets

Platinum single-atom adsorption on graphene: a density functional theory study.

Project description:Single-atom catalysis, which utilizes single atoms as active sites, is one of the most promising ways to enhance the catalytic activity and to reduce the amount of precious metals used. Platinum atoms deposited on graphene are reported to show enhanced catalytic activity for some chemical reactions, e.g. methanol oxidation in direct methanol fuel cells. However, the precise atomic structure, the key to understand the origin of the improved catalytic activity, is yet to be clarified. Here, we present a computational study to investigate the structure of platinum adsorbed on graphene with special emphasis on the edges of graphene nanoribbons. By means of density functional theory based thermodynamics, we find that single platinum atoms preferentially adsorb on the substitutional carbon sites at the hydrogen terminated graphene edge. The structures are further corroborated by the core level shift calculations. Large positive core level shifts indicate the strong interaction between single Pt atoms and graphene. The atomistic insight obtained in this study will be a basis for further investigation of the activity of single-atom catalysts based on platinum and graphene related materials.

| S-EPMC9417699 | biostudies-literature

Copper-Based Catalysts for Selective Hydrogenation of Acetylene Derived from Cu(OH)2.

Project description:Replacing precious metals with cheap metals in catalysts is a topic of interest in both industry and academia but challenging. Here, a selective hydrogenation catalyst was prepared by thermal treatment of Cu(OH)2 nanowires with acetylene-containing gas at 120 °C followed by hydrogen reduction at 150 °C. The characterization by means of transmission electron microscopy observation, X-ray diffraction, and X-ray photoelectron spectroscopy revealed that two crystallites were present in the resultant catalyst. One of the crystal phases was metal Cu, whereas the other crystal phase was ascribed to an interstitial copper carbide (Cu x C) phase. The reduction of freshly prepared copper (II) acetylide (CuC2) at 150 °C also afforded the formation of Cu and Cu x C crystallites, indicating that CuC2 was the precursor or an intermediate in the formation of Cu x C. The prepared catalysts consisting of Cu and Cu x C exhibited a considerably high hydrogenation activity at low temperatures in the selective hydrogenation of acetylene in the ethylene stream. In the presence of a large excess of ethylene, acetylene was completely converted at 110 °C and atmospheric pressure with an ethane selectivity of <15%, and the conversion and selectivity were constant in a 260 h run.

| S-EPMC7860242 | biostudies-literature

Pd/MCM-41 catalyst for acetylene hydrogenation to ethylene.

Project description:This study aims to produce ethylene using the calcium carbide route, acetylene from calcium carbide and then selective hydrogenation of the high-concentration acetylene to ethylene. A series of catalysts with different supports, such as Al2O3, SiO2 and MCM-41, were prepared using the ethylene glycol reduction method and their catalytic properties for high-concentration acetylene hydrogenation of calcium carbide to ethylene were studied by transmission electron microscopy, X-ray powder diffraction and thermogravimetry, among others. The results show that the small particle size and uniform dispersion of palladium (Pd) particles in the Pd/MCM-41 catalyst produced the highest ethylene yield of 62.09%. Then, the conditions for the basic reaction, such as reaction temperature and space velocity, were optimized using MCM-41 as a support. The yield of ethylene after condition optimization was as high as 82.87%, while the loading of Pd was 0.1%.

| S-EPMC6894548 | biostudies-literature

Highly-efficient RuNi single-atom alloy catalysts toward chemoselective hydrogenation of nitroarenes.

Project description:The design and exploitation of high-performance catalysts have gained considerable attention in selective hydrogenation reactions, but remain a huge challenge. Herein, we report a RuNi single atom alloy (SAA) in which Ru single atoms are anchored onto Ni nanoparticle surface via Ru-Ni coordination accompanied with electron transfer from sub-surface Ni to Ru. The optimal catalyst 0.4% RuNi SAA exhibits simultaneously improved activity (TOF value: 4293 h-1) and chemoselectivity toward selective hydrogenation of 4-nitrostyrene to 4-aminostyrene (yield: >99%), which is, to the best of our knowledge, the highest level compared with reported heterogeneous catalysts. In situ experiments and theoretical calculations reveal that the Ru-Ni interfacial sites as intrinsic active centers facilitate the preferential cleavage of N-O bond with a decreased energy barrier by 0.28 eV. In addition, the Ru-Ni synergistic catalysis promotes the formation of intermediates (C8H7NO* and C8H7NOH*) and accelerates the rate-determining step (hydrogenation of C8H7NOH*).

| S-EPMC9178046 | biostudies-literature

Highly efficient ethylene production via electrocatalytic hydrogenation of acetylene under mild conditions.

Project description:Renewable energy-based electrocatalytic hydrogenation of acetylene to ethylene (E-HAE) under mild conditions is an attractive substitution to the conventional energy-intensive industrial process, but is challenging due to its low Faradaic efficiency caused by competitive hydrogen evolution reaction. Herein, we report a highly efficient and selective E-HAE process at room temperature and ambient pressure over the Cu catalyst. A high Faradaic efficiency of 83.2% for ethylene with a current density of 29 mA cm-2 is reached at -0.6 V vs. the reversible hydrogen electrode. In-situ spectroscopic characterizations combined with first-principles calculations reveal that electron transfer from the Cu surface to adsorbed acetylene induces preferential adsorption and hydrogenation of the acetylene over hydrogen formation, thus enabling a highly selective E-HAE process through the electron-coupled proton transfer mechanism. This work presents a feasible route for high-efficiency ethylene production from E-HAE.

| S-EPMC8648715 | biostudies-literature

Metallofullerenes as Robust Single-Atom Catalysts for Adsorption and Dissociation of Hydrogen Molecules: A Density Functional Study.

Project description:Hydrogen is currently considered as the best alternative for traditional fuels due to its sustainable and ecofriendly nature. Additionally, hydrogen dissociation is a critical step in almost all hydrogenation reactions, which is crucial in industrial chemical production. A cost-effective and efficient catalyst with favorable activity for this step is highly desirable. Herein, transition-metal-doped fullerene (TM@C60) complexes are designed and investigated as single-atom catalysts for the hydrogen splitting process. Interaction energy analysis (Eint) is also carried out to demonstrate the stability of designed TM@C60 metallofullerenes, which reveals that all the designed complexes have higher thermodynamic stability. Furthermore, among all the studied metallofullerenes, the best catalytic efficiency for hydrogen dissociation is seen for the Sc@C60 catalyst Ea = 0.13 eV followed by the V@C60 catalyst Ea = 0.19 eV. The hydrogen activation and dissociation processes over TM@C60 metallofullerenes is further elaborated by analyzing charge transfer via the natural bond orbital and electron density difference analyses. Additionally, quantum theory of atoms in molecule analysis is carried out to investigate the nature of interatomic interactions between hydrogen molecules and TMs@C60 metallofullerenes. Overall, results of the current study declare that the Sc@C60 catalyst can act as a low cost, highly efficient, and noble metal-free single-atom catalyst to efficiently catalyze hydrogen dissociation reaction.

| S-EPMC10552115 | biostudies-literature

A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation.

Project description:Preparation of single atom catalysts (SACs) is of broad interest to materials scientists and chemists but remains a formidable challenge. Herein, we develop an efficient approach to synthesize SACs via a precursor-dilution strategy, in which metalloporphyrin (MTPP) with target metals are co-polymerized with diluents (tetraphenylporphyrin, TPP), followed by pyrolysis to N-doped porous carbon supported SACs (M1/N-C). Twenty-four different SACs, including noble metals and non-noble metals, are successfully prepared. In addition, the synthesis of a series of catalysts with different surface atom densities, bi-metallic sites, and metal aggregation states are achieved. This approach shows remarkable adjustability and generality, providing sufficient freedom to design catalysts at atomic-scale and explore the unique catalytic properties of SACs. As an example, we show that the prepared Pt1/N-C exhibits superior chemoselectivity and regioselectivity in hydrogenation. It only converts terminal alkynes to alkenes while keeping other reducible functional groups such as alkenyl, nitro group, and even internal alkyne intact.

| S-EPMC6694111 | biostudies-literature

Thermally stable single atom Pt/m-Al2O3 for selective hydrogenation and CO oxidation.

Project description:Single-atom metal catalysts offer a promising way to utilize precious noble metal elements more effectively, provided that they are catalytically active and sufficiently stable. Herein, we report a synthetic strategy for Pt single-atom catalysts with outstanding stability in several reactions under demanding conditions. The Pt atoms are firmly anchored in the internal surface of mesoporous Al2O3, likely stabilized by coordinatively unsaturated pentahedral Al3+ centres. The catalyst keeps its structural integrity and excellent performance for the selective hydrogenation of 1,3-butadiene after exposure to a reductive atmosphere at 200?°C for 24?h. Compared to commercial Pt nanoparticle catalyst on Al2O3 and control samples, this system exhibits significantly enhanced stability and performance for n-hexane hydro-reforming at 550?°C for 48?h, although agglomeration of Pt single-atoms into clusters is observed after reaction. In CO oxidation, the Pt single-atom identity was fully maintained after 60 cycles between 100 and 400?°C over a one-month period.

| S-EPMC5537564 | biostudies-literature

One-Step High-Temperature-Synthesized Single-Atom Platinum Catalyst for Efficient Selective Hydrogenation.

Project description:Although single-atom catalysts significantly improve the atom utilization efficiency, the multistep preparation procedures are complicated and difficult to control. Herein, we demonstrate that one-step in situ synthesis of the single-atom Pt anchored in single-crystal MoC (Pt1/MoC) by using facile and controllable arc-discharge strategy under extreme conditions. The high temperature (up to 4000°C) provides the sufficient energy for atom dispersion and overall stability by forming thermodynamically favourable metal-support interactions. The high-temperature-stabilized Pt1/MoC exhibits outstanding performance and excellent thermal stability as durable catalyst for selective quinoline hydrogenation. The initial turnover frequency of 3710 h-1 is greater than those of previously reported samples by an order of magnitude under 2 MPa H2 at 100°C. The catalyst also shows broad scope activity toward hydrogenation containing unsaturated groups of C=C, C=N, and C=O. The facile, one-step, and fast arc-discharge method provides an effective avenue for single-atom catalyst fabrication that is conventionally challenging.

| S-EPMC7206892 | biostudies-literature

Controllable Deposition of Bi onto Pd for Selective Hydrogenation of Acetylene.

Project description:The rational regulation of catalyst active sites at atomic scale is a key approach to unveil the relationship between structure and catalytic performance. Herein, we reported a strategy for the controllable deposition of Bi on Pd nanocubes (Pd NCs) in the priority order from corners to edges and then to facets (Pd NCs@Bi). The spherical aberration-corrected scanning transmission electron microscopy (ac-STEM) results indicated that Bi2O3 with an amorphous structure covers the specific sites of Pd NCs. When only the corners and edges of the Pd NCs were covered, the supported Pd NCs@Bi catalyst exhibited an optimal trade-off between high conversion and selectivity in the hydrogenation of acetylene to ethylene under ethylene-rich conditions (99.7% C2H2 conversion and 94.3% C2H4 selectivity at 170 °C) with remarkable long-term stability. According to the H2-TPR and C2H4-TPD measurements, the moderate hydrogen dissociation and the weak ethylene adsorption are responsible for this excellent catalytic performance. Following these results, the selectively Bi-deposited Pd nanoparticle catalysts showed incredible acetylene hydrogenation performance, which provides a feasible perspective to design and develop highly selective hydrogenation catalysts for industrial applications.

| S-EPMC10005703 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data