SCOPUS 정보 검색 플랫폼

Journal of the American Chemical Society

Volumn 128, Issue 51, 2006, Pages 17033-17042

Reduction of O2 to superoxide anion (O2.-) in water by heteropolytungstate cluster-anions

(4) Geletii, Yurii V a Hill, Craig L a Atalla, Rajai H b Weinstock, Ira A c,d

a EMORY UNIVERSITY (United States)

b FOREST PRODUCTS LABORATORY (United States)

c CITY COLLEGE OF NEW YORK (United States)

d BEN GURION UNIVERSITY OF THE NEGEV (Israel)

Author keywords

[No Author keywords available]

Indexed keywords

CATALYSIS; ELECTRON TRANSITIONS; NEGATIVE IONS; OXYGEN; REACTION KINETICS; REDUCTION;

DONOR ION CHARGES; ELECTRON TRANSFER; HETEROPOLYTUNGSTATE CLUSTER ANIONS; SUPEROXIDE ANIONS;

TUNGSTEN COMPOUNDS;

ANION; OXYGEN; SUPEROXIDE; TUNGSTEN DERIVATIVE; WATER; HYDROGEN PEROXIDE;

ANION TRANSPORT; ARTICLE; CATALYSIS; ELECTRON TRANSPORT; ION EXCHANGE; IONIC STRENGTH; ISOTOPE LABELING; PROTON COUPLED ELECTRON TRANSPORT; REDUCTION KINETICS; SOLVENT EFFECT; CHEMISTRY; KINETICS; OXIDATION REDUCTION REACTION;

ANIONS; ELECTRON TRANSPORT; HYDROGEN PEROXIDE; KINETICS; OXIDATION-REDUCTION; OXYGEN; SUPEROXIDES; TUNGSTEN COMPOUNDS; WATER;

EID: 33845941436 PISSN: 00027863 EISSN: None Source Type: Journal
DOI: 10.1021/ja064244g Document Type: Article

Times cited : (69)

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56
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- The k22 values that, when used in the Marcus cross relation, bring calculated rate constants, k12(calcd, fully into line with (identical to) observed k12 values are 3.1, 0.17. and 0.40 kcal mol-1, respectively, for reactions of 1red, 2red, and 3red. These specific k22 values are of questionable utility. This is because, while the small k22 value (2 M-1 mol -1) used in Figure 4 compensates for the difference in size (radii) between reacting species, this size difference is the same for all three Keggin-anion/O2 combinations. Therefore, k22 should, in principal, be the same for all three reactions. That this is not the case likely points to uncertainty in the effective radius of O 2 used to calculate the work terms, wij, in eq 16
- ij, in eq 16.

74
- 0004285028
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- MacInnes, D. A. The Principles of Electrochemistry, 1st ed.; Dover Publications, Inc.: New York, 1961.
- (1961) The Principles of Electrochemistry
- MacInnes, D.A.¹

75
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- Meyer, T. J.; Taube, H. J. Chem. Phys. 1968, 7, 2369-2379.
- (1968) J. Chem. Phys , vol.7 , pp. 2369-2379
- Meyer, T.J.¹ Taube, H.²

76
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- Stanbury, D. M.; Haas, O.; Taube, H. Inorg. Chem. 1980, 19, 518-524.
- (1980) Inorg. Chem , vol.19 , pp. 518-524
- Stanbury, D.M.¹ Haas, O.² Taube, H.³

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- (1999) J. Am. Chem. Soc , vol.121 , pp. 11855-11863
- Anderson, A.B.¹ Albu, T.V.²

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- Studies designed to better understand this are in progress. A key prerequisite (and challenge) is to fully define and control the protonation states of highly charged cluster anions at low pH values in water
- Studies designed to better understand this are in progress. A key prerequisite (and challenge) is to fully define and control the protonation states of highly charged cluster anions at low pH values in water.

79
- 32544458992
- While the W12O36 shells of 1, 2, and 3, are isostructural, Xn+-μ4-O and μ4-O-W bond distances vary slightly with heteroatom size and electronegativity. This accounts for the variation in λ values. See Sundaram, K. M, Neiwert, W. A, Hill, C. L, Weinstock, I. A. Inorg. Chem. 2006, 45, 958-960
- 4-O-W bond distances vary slightly with heteroatom size and electronegativity. This accounts for the variation in λ values. See Sundaram, K. M.; Neiwert, W. A.; Hill, C. L.; Weinstock, I. A. Inorg. Chem. 2006, 45, 958-960.

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- -1.
- -1.

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- As noted above, the increase in λ values also contributes to the leveling of k12 values. For example, estimates indicate that if λ for a self-exchange between 1red and 1 oz were equal to that associated with exchange between reduced and oxidized forms of 3 (i.e, 25.2 kcal mol-1, the observed rate constant, k12, for reaction of 1 red with O2 would increase by an amount similar to that obtained by setting w21, 0 in Figure 6. However, the effect of variation in charge is much more significant: (1) it provides support for the ET-PT mechanism, 2) it is generally applicable to all outersphere reactions of charged donors with O2, and (3) it is rarely observed, let alone quantified. In this regard, it bears noting that all values in Figure 6 are calculated using experimental k11 values, and therefore, the
- 11 values, and therefore, the results are entirely independent of the underlying variation in λ values.

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- +] values varied by nearly 0.5 M). That work is reviewed in ref 14.
- +] values varied by nearly 0.5 M). That work is reviewed in ref 14.

83
- 85099526230
- 2- anion and 0.74 Å for 6-coordinate W(VI): from Huheey, J. E. Inorganic Chemistry: Principles of Structure and Reactivity, 2nd ed.; Harper and Row: New York, 1978.
- 2- anion and 0.74 Å for 6-coordinate W(VI): from Huheey, J. E. Inorganic Chemistry: Principles of Structure and Reactivity, 2nd ed.; Harper and Row: New York, 1978.

* 이 정보는 Elsevier사의 SCOPUS DB에서 KISTI가 분석하여 추출한 것입니다.