TY - JOUR
T1 - Controllable Synthesis and Catalytic Performance of Nanocrystals of Rare-Earth-Polyoxometalates
AU - Li, Shujun
AU - Zhou, Yanfang
AU - Peng, Qingpo
AU - Wang, Ruoya
AU - Feng, Xiaoge
AU - Liu, Shuxia
AU - Ma, Xiaoming
AU - Ma, Nana
AU - Zhang, Jie
AU - Chang, Yi
AU - Zheng, Zhiping
AU - Chen, Xuenian
N1 - Funding Information:
This work was supported by the National Natural Science Foundation of China (Grant Nos. 21401047, 21371029, 21603062, and 21771057), the China Postdoctoral Science Foundation (No. 2017M622350), the Open Research Fund of Henan Key Laboratory of Polyoxometalate Chemistry, (HNPOMKF1702), Key Program for High School of Henan Province (16A150012), and the Shenzhen Nobel Prize Scientists Laboratory Project (C17213101). All calculations were supported by the High Performance Computing Center of Henan Normal University.
Publisher Copyright:
© 2018 American Chemical Society.
PY - 2018/6/4
Y1 - 2018/6/4
N2 - Large-scale isolation of nanocrystals of rare-earth-polyoxometalates (RE-POMs) catalysts is important in fundamental research and applications. Here, we synthesized a family of monomeric RE-POMs by the self-assembly of Ta/W mixed-addendum POM {P2W15Ta3O62} and rare-earth (RE) ions. These RE-POMs with molecular formulas of [RE(H2O)7]3P2W15Ta3O62·nH2O (RE = Y, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu) are all electroneutral molecular clusters, insoluble in water and common organic solvents. The electronic structures, electrochemical properties, and catalytic activities of them have been investigated by experimental and computational methods. In particular, based on a mild and controllable synthetic process, a convenient and controllable approach to prepare nanocrystals and self-organized aggregates of these monomers has been developed. They exhibit remarkable heterogeneous catalytic activity for cyanosilylation. Both the increased Lewis acid strength of RE in the title compounds, as indicated by theoretical calculations, and the decreased particle size contribute to their high catalytic performances.
AB - Large-scale isolation of nanocrystals of rare-earth-polyoxometalates (RE-POMs) catalysts is important in fundamental research and applications. Here, we synthesized a family of monomeric RE-POMs by the self-assembly of Ta/W mixed-addendum POM {P2W15Ta3O62} and rare-earth (RE) ions. These RE-POMs with molecular formulas of [RE(H2O)7]3P2W15Ta3O62·nH2O (RE = Y, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, and Lu) are all electroneutral molecular clusters, insoluble in water and common organic solvents. The electronic structures, electrochemical properties, and catalytic activities of them have been investigated by experimental and computational methods. In particular, based on a mild and controllable synthetic process, a convenient and controllable approach to prepare nanocrystals and self-organized aggregates of these monomers has been developed. They exhibit remarkable heterogeneous catalytic activity for cyanosilylation. Both the increased Lewis acid strength of RE in the title compounds, as indicated by theoretical calculations, and the decreased particle size contribute to their high catalytic performances.
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U2 - 10.1021/acs.inorgchem.8b00763
DO - 10.1021/acs.inorgchem.8b00763
M3 - Article
AN - SCOPUS:85048305176
SN - 0020-1669
VL - 57
SP - 6624
EP - 6631
JO - Inorganic Chemistry
JF - Inorganic Chemistry
IS - 11
ER -