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Yakovlev, A.L.; Zhidomirov, G. M.

doi:10.1023/a:1019092232161

Cited by 12 publications

(8 citation statements)

References 23 publications

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“…The hydroxylated form of a binuclear Fe center acts as a single Fe site. This conclusion is in agreement with the results of DFT calculations [28], which showed that the hydroxylated form of a binuclear Fe center consists of one Fe ion completely saturated by water in the first coordination sphere. The result with H 2 O blocking one-half of the Fe atoms also indirectly confirms the presence of proton in the binuclear diamond core, since otherwise two molecules of H 2 O could be accommodated during adsorption on a [Fe 2 O 2 ] 2+ center.…”

Section: Discussionsupporting

confidence: 92%

“…This is in line with the prediction by DFT analysis for a terminal Fe-O group distance of 1.61 Å, indicating strong double-bond character [28]. We assume that CO interacts with the active terminal oxygen atoms forming CO 2 .…”

Section: Discussionsupporting

confidence: 91%

“…In these cases, besides an active binuclear Fe complex, other forms of iron may be present, as was confirmed experimentally. Combining these results with recent theoretical studies [27][28][29], a tentative structure for the active center and its formation can be proposed.…”

Section: Discussionsupporting

confidence: 53%

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Active sites in HZSM-5 with low Fe content for the formation of surface oxygen by decomposing N2O: is every deposited oxygen active?

Kiwi‐Minsker

2003

Journal of Catalysis

131

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Surface-active centers were detected in HZSM-5 with a low content of iron (< 1000 ppm) activated by steaming and high-temperature calcination in inert atmospheres (up to 1323 K). These centers lead to the formation of surface oxygen (O) ad species from N 2 O and were characterized quantitatively by the transient response method. The total amount of active centers was proportional to the content of iron in the zeolites. Only a part of (O) ad deposited by decomposing N 2 O was active in CO oxidation at 523 K and appeared as sharp O 2 peaks at 666 K during the TPD measurements. A binuclear Fe center is suggested featuring a "diamond core" structure, similar to that of the monooxygenase enzyme, as an active center. The active O atoms were assigned to the paired terminal oxygen atoms each bonded to one Fe site (ferryl groups) in the diferric [Fe 2 O 2 H] + cluster. Oxygen pretreatment at 823 K decreases somewhat the total amount of active sites but does not affect the ratio of active/inactive oxygen. Zeolite presaturated by water vapor at 473-523 K generates (O) ad species from N 2 O completely inactive in the CO oxidation. Part of it appears as a broad peak at 940 K in the TPD profile. The total amount of the deposited oxygen corresponds to half of the stoichiometric amount of the surface Fe atoms and suggests that water blocks a half of the binuclear [Fe 2 O 2 H] + center, the remaining acting as a single Fe site.

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Section: Discussionsupporting

confidence: 92%

Section: Discussionsupporting

confidence: 91%

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Active sites in HZSM-5 with low Fe content for the formation of surface oxygen by decomposing N2O: is every deposited oxygen active?

Kiwi‐Minsker

2003

Journal of Catalysis

131

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“…And the first step is more pivotal, which is focused on by most scholars. It is interesting that Al has been found similar catalytic effect with noble metals by A. L. Yakovelv et al 5 . Platinum heavy metals [11][12][13][14][15][16] and some transition metals 17,18 could effectively decompose N 2 O with a relatively low barrier.…”

Section: Introductionmentioning

confidence: 81%

“…It is a two-step mechanism that includes N 2 O / N 2 + O followed by N 2 O + O / N 2 + O 2 , and the rst step, which is focused on by most scholars, is more pivotal. 5,6 In order to overcome the high energy barrier of N 2 O decomposition, 7-10 plenty of studies have been done to nd out appropriate catalysts. Platinum heavy metals [11][12][13][14][15][16] and some transition metals 17,18 could effectively decompose N 2 O with a relatively low barrier.…”

Section: Introductionmentioning

confidence: 99%

The effective adsorption and decomposition of N₂O on Al-decorated graphene oxide under electric field

Chen

et al. 2015

RSC Adv.

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The adsorption property and decomposition process of N 2 O molecule on Al-decorated graphene oxide (Al@GO) are investigated by using first-principles calculations. The physical adsorbed N 2 O could be decomposed to N 2 molecule and O atom bonded on Al@GO exothermally (2.33 eV per N 2 O molecule), indicating a stronger interaction of Al cation and O anion of N 2 O. This interaction will be enhanced with a positive external electric field, inducing the corresponding higher binding energy and shortened d Al-O . The decomposition barrier of N 2 O on Al@GO is about 0.50 eV. Especially, for the elongated d Al-O and shortened d O-N1 in transition state, the decomposition barrier is also decreased monotonously with the increasing electric field. It is remarkable that the N 2 O decomposition process becomes almost unimpeded and spontaneous under a positive electric field of 0.50 V/Å. Al-decorated graphene oxide is expected as a new promising candidate for N 2 O decomposition with enhanced adsorption and easier decomposition process. enhance the interaction between N 2 O molecule and Al@GO. Meanwhile, as shown in Figure 3 (b), the corresponding d Al-O is monotonously shortened from 3.24 Å to 2.09 Å and d O-N1 is lengthened from 1.19 Å to 1.24 Å, indicating an enhanced interaction of Al atom and O atom with increasing E.Figure 3. (a) The binding energies of N 2 O on Al@GO, (b) d Al-O and d O-N1 , (c) the bader charges of Al atom and O atom in adsorbed states under different electric fields. The legend is the same as Figure 2. The variations of binding energy and the bond length could be resulted from two dominant factors: the interaction between inherent electric dipole P with E and the charge redistribution induced by E. The formula W= −P×E means a stronger interaction with increasing E. On the other hand, according to bader charge analysis, the charge of O atom is almost unchanged at the beginning, while the charge of AlFigure 5. PDOS of IS, TS and FS during N 2 O decomposition process on the Al@GO system. The legend is the same as Figure 2.Figure 6. (a) The binding energies, (b) d Al-O and d O-N1 in decomposed states under different electric fields. The legend is the same as Figure 2.Figure 7. The decomposition barriers and IS, TS, FS under different electric fields. The legend is the same as Figure 2.

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Identification of Active Oxygen Species over Fe Complexes in Zeolites

Panov

Дубков

Paukshtis

2001

Catalysis by Unique Metal Ion Structures in Solid Matrices

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Untitled

Cited by 12 publications

References 23 publications

Active sites in HZSM-5 with low Fe content for the formation of surface oxygen by decomposing N2O: is every deposited oxygen active?

Active sites in HZSM-5 with low Fe content for the formation of surface oxygen by decomposing N2O: is every deposited oxygen active?

The effective adsorption and decomposition of N₂O on Al-decorated graphene oxide under electric field

Identification of Active Oxygen Species over Fe Complexes in Zeolites

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Untitled

Cited by 12 publications

References 23 publications

Active sites in HZSM-5 with low Fe content for the formation of surface oxygen by decomposing N2O: is every deposited oxygen active?

Active sites in HZSM-5 with low Fe content for the formation of surface oxygen by decomposing N2O: is every deposited oxygen active?

The effective adsorption and decomposition of N2O on Al-decorated graphene oxide under electric field

Identification of Active Oxygen Species over Fe Complexes in Zeolites

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The effective adsorption and decomposition of N₂O on Al-decorated graphene oxide under electric field