Understanding complete oxidation of methane on spinel oxides at a molecular level

Tao, Franklin Feng; Shan, Junjun; Nguyễn, Luân; Wang, Ziyun; Zhang, Shiran; Zhang, Li; Wu, Zili; Huang, Weixin; Zeng, Shibi; Hu, P.

doi:10.1038/ncomms8798

Cited by 268 publications

(225 citation statements)

References 47 publications

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“…In situ studies of surface chemistry of these catalysts were performed on the ambient pressure XPS using monochromated Al Ka in the Tao group 11,29,30 . The binding energy of catalyst samples were calibrated to Au 4f 7/2 at 84.0 eV and Ag 3d 5/2 at 368.3 eV (ref.…”

Section: Methodsmentioning

confidence: 99%

Catalysis on singly dispersed bimetallic sites

et al. 2015

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A catalytic site typically consists of one or more atoms of a catalyst surface that arrange into a configuration offering a specific electronic structure for adsorbing or dissociating reactant molecules. The catalytic activity of adjacent bimetallic sites of metallic nanoparticles has been studied previously. An isolated bimetallic site supported on a non-metallic surface could exhibit a distinctly different catalytic performance owing to the cationic state of the singly dispersed bimetallic site and the minimized choices of binding configurations of a reactant molecule compared with continuously packed bimetallic sites. Here we report that isolated Rh 1 Co 3 bimetallic sites exhibit a distinctly different catalytic performance in reduction of nitric oxide with carbon monoxide at low temperature, resulting from strong adsorption of two nitric oxide molecules and a nitrous oxide intermediate on Rh 1 Co 3 sites and following a low-barrier pathway dissociation to dinitrogen and an oxygen atom. This observation suggests a method to develop catalysts with high selectivity.

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Section: Methodsmentioning

confidence: 99%

Catalysis on singly dispersed bimetallic sites

et al. 2015

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“…For instance, a recent study has shown that NCO can completely oxidize methane to CO 2 and water in the temperature range of 350-550 C 7 . Considering that NCO is also a cheap material made of earth-abundant elements, this result suggests that NCO may be a better methane oxidation catalyst than typical precious-metal-based catalysts 8 .…”

Section: Introductionmentioning

confidence: 99%

“…various bulk 13,19 and surface 7,20 properties have been investigated, but many aspects of the behavior of this material, e.g. the origin of the half-metallic ferrimagnetic structure and the influence of oxygen vacancies, are still largely unexplored.…”

Section: Introductionmentioning

confidence: 99%

“…Nickel cobaltite NiCo 2 O 4 (NCO) is an emerging technological material with a variety of promising applications, ranging from supercapacitors 1-4 to catalysts for CH 4 and low temperature CO oxidation [5][6][7] . For instance, a recent study has shown that NCO can completely oxidize methane to CO 2 and water in the temperature range of 350-550 C 7 .…”

Section: Introductionmentioning

confidence: 99%

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Formation, Electronic Structure, and Defects of Ni Substituted Spinel Cobalt Oxide: a DFT+U Study

2016

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Nickel substituted spinel cobalt oxide is a promising technological material with complex electronic and magnetic structures. Understanding these structures is important for improving the material's performance in various applications. We have carried out first principles calculations on the formation, electronic properties and defects of bulk NiCo 2 O 4 using density functional theory (DFT) with on-site Hubbard U terms on the transition metal d states. Analysis of the electronic structure of Ni x Co 3-x O 4 as a function of x= 0 -1 shows that Ni acts as a p-type dopant in Co 3 O 4 , gradually transforming the minority spin channel from insulating to conducting. As a result, the inverse spinel NiCo 2 O 4 (NCO) is found to have a ferrimagnetic half-metallic ground state with fractional valence on Ni and Co cations at tetrahedral sites (Td), in agreement with experimental observations. Projected Densities of States confirm that the states around the Fermi energy originate from Ni and Co(Td) 3d states hybridized with oxygen 2p orbitals. The influence of two common defects, Ni↔Co(Td) exchanges and oxygen vacancies, on the structural and electronic properties has been also investigated. Our results are consistent with the experimental observation that intermediate structures between inverse spinel and normal spinel occur frequently in NCO. Oxygen vacancies are predicted to occur more frequently at sites coordinated to a larger number of Ni ions and found to have only minor effects on the conductivity and magnetic structure.

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“…To answer this question, we examined the CO adsorption energies on the one-atom substituted Pt alloy surfaces. This system was chosen due to the following reasons: Firstly, the adsorption of CO is very important in many reactions such as CO oxidation 37,40 , dry reforming 38 , CO 2 reduction 41 , and methane oxidation 42 . Secondly, CO adsorbs on the top site of Pt(111), which can also test the generality of the BCCF.…”

Section: Resultsmentioning

confidence: 99%

Formulating the bonding contribution equation in heterogeneous catalysis: a quantitative description between the surface structure and adsorption energy

Wang

2017

Phys. Chem. Chem. Phys.

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The relation between surface structure and adsorption energy of adsorbate is of great importance in heterogeneous catalysis. Based on density functional theory calculations, we propose an explicit equation with three chemically meaningful terms, namely the bonding contribution equation, to quantitatively account the surface structures and the adsorption energies. Successful predictions of oxygen adsorption energies on complex alloy surfaces containing up to 4 components are demonstrated, and the generality of this equation is also tested using different surface sizes and other adsorbates. This work not only may offer a powerful tool to understand the structureadsorption relation, but also may be used to inversely design novel catalysts.

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Understanding complete oxidation of methane on spinel oxides at a molecular level

Cited by 268 publications

References 47 publications

Catalysis on singly dispersed bimetallic sites

Catalysis on singly dispersed bimetallic sites

Formation, Electronic Structure, and Defects of Ni Substituted Spinel Cobalt Oxide: a DFT+U Study

Formulating the bonding contribution equation in heterogeneous catalysis: a quantitative description between the surface structure and adsorption energy

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