{Ta12}/{Ta16) Cluster-Containing Polytantalotungstates with Remarkable Photocatalytic H2 Evolution Activity

被引：161

作者：

Li, Shujun ^{[1
]}

Liu, Shumei ^{[1
,2
]}

Liu, Shuxia ^{[1
]}

Liu, Yiwei ^{[1
]}

Tang, Qun ^{[1
]}

Shi, Zhan ^{[3
]}

Ouyang, Shuxin ^{[4
]}

Ye, Jinhua ^{[4
]}

机构：

[1] NE Normal Univ, Coll Chem, Minist Educ, Key Lab Polyoxometalate Sci, Changchun 130024, Jilin, Peoples R China

[2] Jilin Univ, Dept Mat Sci & Engn, Changchun 130025, Peoples R China

[3] Jilin Univ, Coll Chem, State Key Lab Inorgan Synth & Preparat Chem, Changchun 130012, Peoples R China

[4] Natl Inst Mat Sci, Photocatalyt Mat Ctr PCMC, Tsukuba, Ibaraki 3050047, Japan

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2012年 / 134卷 / 48期

关键词：

METAL-OXIDE ANALOGS; NATAO3; PHOTOCATALYSTS; PHOTOREDOX CHEMISTRY; WATER DECOMPOSITION; MOLECULAR-STRUCTURE; HYDROGEN-PRODUCTION; DOPED NATAO3; SOLID-STATE; POLYOXOMETALATE; OXIDATION;

D O I：

10.1021/ja307484a

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Four novel polytantalotungstates K5Na4[P2W15O59 (TaO2)(3)]center dot 17H(2)O(1), K8Na8H4[P8W60Ta12(H2O)(4)(OH)(8)O-236]center dot 42H(2)O(2), Cs3K3.5H0.5[SiW9(TaO2)(3)O-37]center dot 9H(2)O(3), and Cs10.5K4H5.5[Ta4O6(SiW9Ta3O40)(4)]center dot 30H(2)O(4) were synthesized. Compounds 1 and 3 are tris-(peroxotantalum)-substituted Dawson- and Keggin-type derivatives, whereas 2 and 4 are teerameric oligomers containing respectively an unprecedented {Ta-12} and {Ta-16} cluster core. The photocatalytic activities of 2 and 4 for H-2 evolution from water were evaluated. The significantly enhanced performance against the control K-6 [P2W18O62] can be attributed to the modulation of the electronic structures of these novel POMs by Ta incorporation. The highest activity observed so far with the use of 2 can be further rationalized by the presence of distorted heptacoordinate Ta atoms in the form of TaO7 pentagonal bipyramid.

引用

页码：19716 / 19721

页数：6

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