scholarly journals Novel structure of active platinum-bismuth site for oxidation of carbon monoxide

2020 ◽  
Author(s):  
Bing Nan ◽  
Qiang Fu ◽  
Miao Shu ◽  
Lulu Zhou ◽  
Wei-Wei Wang ◽  
...  
Keyword(s):  
Carbon Monoxide ◽  
Low Temperature ◽  
Co Oxidation ◽  
Density Functional ◽  
Technology Development ◽  
Co Adsorption ◽  
Advanced Combustion ◽  
Novel Structure ◽  
Surface Metal ◽  
Bismuth Cluster

Abstract As the technology development, the future advanced combustion engines must be designed to perform at a low temperature. Thus, it is a great challenge to synthesize high active and stable catalysts to resolve exhaust below 100 °C. Here, we report that bismuth as a dopant added to form platinum-bismuth cluster on silica for CO oxidation. The highly reducible oxygen species provided by surface metal-oxide (M-O) interface could be activated by CO at low temperature (~ 50 °C) with a high CO2 production rate of 487 µmolCO2·gPt−1·s− 1 at 110 °C. Experiment data combined with density functional calculation (DFT) results demonstrate that Pt cluster with surface Pt−O−Bi structure is the active site for CO oxidation via providing moderate CO adsorption and activating CO molecules with electron transformation between platinum atom and carbon monoxide. These findings provide a novel and general approach towards design of potential outstanding performance catalysts for redox reaction.

scholarly journals Unique structure of active platinum-bismuth site for oxidation of carbon monoxide

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Bing Nan ◽  
Qiang Fu ◽  
Jing Yu ◽  
Miao Shu ◽  
Lu-Lu Zhou ◽  
...  
Keyword(s):  
Carbon Monoxide ◽  
Low Temperature ◽  
Co Oxidation ◽  
Density Functional ◽  
Technology Development ◽  
Co Adsorption ◽  
Combustion Engines ◽  
Advanced Combustion ◽  
Surface Metal ◽  
Bismuth Cluster

AbstractAs the technology development, the future advanced combustion engines must be designed to perform at a low temperature. Thus, it is a great challenge to synthesize high active and stable catalysts to resolve exhaust below 100 °C. Here, we report that bismuth as a dopant is added to form platinum-bismuth cluster on silica for CO oxidation. The highly reducible oxygen species provided by surface metal-oxide (M-O) interface could be activated by CO at low temperature (~50 °C) with a high CO2 production rate of 487 μmolCO2·gPt−1·s−1 at 110 °C. Experiment data combined with density functional calculation (DFT) results demonstrate that Pt cluster with surface Pt−O−Bi structure is the active site for CO oxidation via providing moderate CO adsorption and activating CO molecules with electron transformation between platinum atom and carbon monoxide. These findings provide a unique and general approach towards design of potential excellent performance catalysts for redox reaction.

Analysis of Preferred Mechanisms of CO Oxidation with Atomically Dispersed Pt1/TiO2 Using the Energetic Span Model

2021 ◽  
Author(s):  
Selin Bac ◽  
Shaama Mallikarjun Sharada
Keyword(s):  
Low Temperature ◽  
Co Oxidation ◽  
Density Functional ◽  
Co Adsorption ◽  
Ab Initio Molecular Dynamics ◽  
Functional Theory ◽  
Support Materials ◽  
Dispersed Catalysts ◽  
Active Metal ◽  
Low Temperature Co Oxidation

This work examines mechanisms of low-temperature CO oxidation over a single binding site of atomically dispersed Pt on rutile TiO2 (110) using density functional theory and the energetic span model (ESM). Of the 12 distinct pathways spanning Eley- Rideal (ER), termolecular ER (TER), Langmuir-Hinshelwood (LH), Mars-Van Krevelen (MvK) mechanisms as well as their combinations, TER with CO-assisted CO2 desorption yields the highest turnover frequency (TOF). However, this pathway is ruled out because Pt is dynamically unstable in an intermediate state in the TER cycle, determined in a prior ab initio molecular dynamics study by our group. We instead find, depending on reaction conditions, that either H1 is rendered inactive upon CO adsorption or the ER mechanism is preferred if O2 dissociatively adsorbs. ER exhibits the second highest TOF and the TOF-determining state is in qualitative agreement with experiment. TOFs for all MvK pathways are several orders of magnitude lower than ER and LH. By comparing TOFs for Pt1/TiO2 with prior mechanistic studies of various oxide-supported atomically dispersed catalysts in the literature, we identify the most active metal and support materials for low-temperature CO oxidation.

The interplay between structural perfectness and CO oxidation catalysis on aluminum, phosphorous and silicon complexes of corroles

2019 ◽  
Vol 21 (14) ◽  
pp. 7661-7674 ◽  
Author(s):  
Afshan Mohajeri ◽  
Nasim Hassani
Keyword(s):  
Density Functional Theory ◽  
Carbon Monoxide ◽  
Co Oxidation ◽  
Catalytic Oxidation ◽  
Density Functional ◽  
Density Functional Theory Calculations ◽  
Oxidation Catalysis ◽  
Functional Theory ◽  
Oxidation Of Carbon Monoxide

Catalytic oxidation of carbon monoxide on perfect and defective structures of corrole complexes with aluminum, phosphorous and silicon have been investigated by performing density functional theory calculations.

Investigation of Carbon Monoxide Adsorption on Cationic Gold- Palladium Clusters

2013 ◽  
Vol 68 (10-11) ◽  
pp. 651-658 ◽  
Author(s):  
Yang-Mei Chen ◽  
Xiao-Yu Kuang ◽  
Xiao-Wei Sheng ◽  
Huai-Qian Wang ◽  
Peng Shao ◽  
...  
Keyword(s):  
Carbon Monoxide ◽  
Molecular Orbital ◽  
Density Functional ◽  
Co Adsorption ◽  
Vibration Strength ◽  
Au Clusters ◽  
Highest Occupied Molecular Orbital ◽  
Lowest Unoccupied Molecular Orbital ◽  
Pd Clusters ◽  
Homo Lumo

Density functional calculations have been performed for the carbon monoxide molecule adsorption on AunPd+m(n+m ≤ 6) clusters. In the process of CO adsorption, small Au clusters and Pd clusters tend to be an Au atom and three Pd atoms adsorption, respectively. For the mixed Au-Pd clusters, an Au atom, a Pd atom, two atoms consisted of an Au atom and a Pd atom, two Pd atoms, and three Pd atoms adsorption structures are displayed. The highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) gaps and natural bond orbital charge population are calculated. Moreover, CO adsorption energy, CO stretching frequency, and CO bond length (upon adsorption) are also analysed in detail. The results predict that the adsorption strength of Au clusters with CO and the C-O vibration strength is enhanced and reduced after doping of Pd in the AunPdmCO+ complexes, respectively

CeO2 supported low-loading Au as an enhanced catalyst for low temperature oxidation of carbon monoxide

CrystEngComm ◽  
2019 ◽  
Vol 21 (46) ◽  
pp. 7108-7113 ◽  
Author(s):  
Lingling Li ◽  
Yu Liu ◽  
Qishun Wang ◽  
Xuan Zhou ◽  
Jian Li ◽  
...  
Keyword(s):  
Carbon Monoxide ◽  
Low Temperature ◽  
Co Oxidation ◽  
High Activity ◽  
Supported Catalysts ◽  
Coprecipitation Method ◽  
Low Temperature Oxidation ◽  
Temperature Oxidation ◽  
Oxidation Of Carbon Monoxide

A series of low loading and high activity Au/CeO2 supported catalysts were synthesized using a coprecipitation method. Au/CeO2 catalysts with a low Au content (0.2 wt%) showed extremely high activity for CO oxidation with 100% conversion of CO around 60 °C.

Highly active and stable Au@CuxO core–shell nanoparticles supported on alumina for carbon monoxide oxidation at low temperature

RSC Advances ◽  
2016 ◽  
Vol 6 (79) ◽  
pp. 75126-75132 ◽  
Author(s):  
Weining Zhang ◽  
Qingguo Zhao ◽  
Xiaohong Wang ◽  
Xiaoxia Yan ◽  
Sheng Han ◽  
...  
Keyword(s):  
Carbon Monoxide ◽  
Catalytic Activity ◽  
Low Temperature ◽  
Co Oxidation ◽  
Room Temperature ◽  
Core Shell ◽  
Shell Nanoparticles ◽  
Highly Active ◽  
Co Conversion ◽  
Core Shell Nanoparticles

Au@CuxO core–shell nanoparticles and Au@CuxO/Al2O3 used for CO oxidation at low temperature are prepared. CO conversion on Au@CuxO/Al2O3 can reach to 38% at room temperature and the catalytic activity remains unchanged after 108 hours reaction.

First-principles study of nitrogen and carbon monoxide adsorptions on silicene

2016 ◽  
Vol 30 (25) ◽  
pp. 1650176 ◽  
Author(s):  
Shuying Zhong ◽  
Fanghua Ning ◽  
Fengya Rao ◽  
Xueling Lei ◽  
Musheng Wu ◽  
...  
Keyword(s):  
Density Functional Theory ◽  
Carbon Monoxide ◽  
Charge Transfer ◽  
First Principles ◽  
Density Functional ◽  
Co Adsorption ◽  
Functional Theory ◽  
The Density Functional Theory ◽  
Adsorption Energies ◽  
Charge Calculations

Atomic adsorptions of N, C and O on silicene and molecular adsorptions of N2 and CO on silicene have been investigated using the density functional theory (DFT) calculations. For the atomic adsorptions, we find that the N atom has the most stable adsorption with a higher adsorption energy of 8.207 eV. For the molecular adsorptions, we find that the N2 molecule undergoes physisorption while the CO molecule undergoes chemisorption, the corresponding adsorption energies for N2 and CO are 0.085 and 0.255 eV, respectively. Therefore, silicene exhibits more reactivity towards the CO adsorption than the N2 adsorption. The differences of charge density and the integrated charge calculations suggest that the charge transfer for CO adsorption ([Formula: see text]0.015[Formula: see text]) is larger than that for N2 adsorption ([Formula: see text]0.005[Formula: see text]). This again supports that CO molecule is more active than N2 molecule when they are adsorbed onto silicene.

Dissociative Adsorption of O2 on Clean and CO-Precovered Pt Surfaces

2008 ◽  
Vol 1084 ◽  
Author(s):  
Bin Shan ◽  
Ligen Wang ◽  
Jangsuk Hyun ◽  
Yang Sang ◽  
Yujun Zhao ◽  
...  
Keyword(s):  
Co Oxidation ◽  
Density Functional ◽  
Atomic Oxygen ◽  
Activation Barrier ◽  
Co Adsorption ◽  
Dissociative Adsorption ◽  
Binding Energies ◽  
Critical Question ◽  
Oxygen Dissociation ◽  
Langmuir Hinshelwood Mechanism

ABSTRACTIt is generally accepted that CO oxidation on transition metals follows a Langmuir-Hinshelwood mechanism. The oxidation reaction takes place in two sequential steps where the oxygen molecule first dissociates into atomic oxygen and then reacts with an adsorbed CO to form CO2. One critical question concerning the reaction kinetics under high pressure is the probability of oxygen dissociation on a highly CO covered surface. On bare transition metal surfaces, molecularly adsorbed oxygen readily dissociates with little or no apparent activation barrier. In industrial diesel engine catalysis, the metal surface is initially packed with CO. Subsequent reactions such as oxygen dissociation must take place on a CO covered surface. In this paper, we performed density functional theory (DFT) calculations for O2 dissociation on Pt(111) in the presence of different CO adsorption environments. While several stable O2 molecular precursor states (top-bridge-top, top-fcc-bridge, and top-hcp-bridge) exist on a clean Pt(111) surface, these precursors become endothermic beyond a critical CO coverage of ∼0.44 ML. Furthermore, the reaction path for CO oxidation via dissociated atomic oxygen becomes less favorable at higher CO coverage, primarily due to competitive adsorption and lateral repulsion. It was found that the oxygen dissociation barrier and the binding energies of atomic oxygen are well correlated via the Evans-Polanyi relationship.

The role of zirconia in cobaltosic oxide catalysts for low-temperature CO oxidation

RSC Advances ◽  
2016 ◽  
Vol 6 (112) ◽  
pp. 111070-111078 ◽  
Author(s):  
Fan Du ◽  
Guisheng Wu ◽  
Dongsen Mao ◽  
Guanzhong Lu
Keyword(s):  
Low Temperature ◽  
Co Oxidation ◽  
Co Adsorption ◽  
Oxide Catalysts ◽  
Low Temperature Co Oxidation ◽  
Cobaltosic Oxide ◽  
Adsorption Desorption

A series of Co3O4/ZrO2 catalysts for low-temperature CO oxidation was prepared, and then characterized by low-temperature N2 adsorption/desorption, XRD, TEM, XPS, UV-vis, CO-TPR, CO adsorption and CO2 desorption.

scholarly journals Highly Catalytic Electrochemical Oxidation of Carbon Monoxide on Iridium Nanotubes: Amperometric Sensing of Carbon Monoxide

Nanomaterials ◽  
2020 ◽  
Vol 10 (6) ◽  
pp. 1140
Author(s):  
Areum Yu ◽  
Taehui Kwon ◽  
Chongmok Lee ◽  
Youngmi Lee
Keyword(s):  
Carbon Monoxide ◽  
Density Functional ◽  
Co Adsorption ◽  
Linear Sweep Voltammetry ◽  
Density Functional Theory Calculations ◽  
Hydrogen Gas ◽  
Solution Temperature ◽  
Current Response ◽  
Amperometric Sensing ◽  
Metal Nanotubes

The nanotubular structures of IrO2 and Ir metal were successfully synthesized without any template. First, IrO2 nanotubes were prepared by electrospinning and post-calcination, where a fine control of synthetic conditions (e.g., precursor concentration and solvent composition in electrospinning solution, temperature increasing rate for calcination) was required. Then, a further thermal treatment of IrO2 nanotubes under hydrogen gas atmosphere produced Ir metal nanotubes. The electroactivity of the resultant Ir metal nanotubes was investigated toward carbon monoxide (CO) oxidation using linear sweep voltammetry (LSV) and amperometry. The anodic current response of Ir metal nanotubes was linearly proportional to CO concentration change, with a high sensitivity and a short response time. The amperometric sensitivity of Ir metal nanotubes for CO sensing was greater than a nanofibrous counterpart (i.e., Ir metal nanofibers) and commercial Pt (20 wt% Pt loading on carbon). Density functional theory calculations support stronger CO adsorption on Ir(111) than Pt(111). This study demonstrates that metallic Ir in a nanotubular structure is a good electrode material for the amperometric sensing of CO.

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