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Controllable Synthesis and Catalytic Performance of Nanocrystals of Rare-Earth-Polyoxometalates
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2018-05-11 00:00:00 , DOI: 10.1021/acs.inorgchem.8b00763 Shujun Li 1 , Yanfang Zhou 1 , Qingpo Peng 1 , Ruoya Wang 1 , Xiaoge Feng 1 , Shuxia Liu 2 , Xiaoming Ma 1 , Nana Ma 1 , Jie Zhang 1 , Yi Chang 1 , Zhiping Zheng 3 , Xuenian Chen 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2018-05-11 00:00:00 , DOI: 10.1021/acs.inorgchem.8b00763 Shujun Li 1 , Yanfang Zhou 1 , Qingpo Peng 1 , Ruoya Wang 1 , Xiaoge Feng 1 , Shuxia Liu 2 , Xiaoming Ma 1 , Nana Ma 1 , Jie Zhang 1 , Yi Chang 1 , Zhiping Zheng 3 , Xuenian Chen 1
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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.
中文翻译：
稀土多金属氧酸盐纳米晶的可控合成及催化性能
稀土多金属氧酸盐（RE-POMs）催化剂的纳米晶体的大规模分离在基础研究和应用中很重要。在这里，我们通过Ta / W混合齿顶POM {P 2 W 15 Ta 3 O 62 }和稀土（RE）离子的自组装合成了一系列单体RE-POM 。这些分子式为[RE（H 2 O）7 ] 3 P 2 W 15 Ta 3 O 62 · n H 2的RE-POMO（RE = Y，Eu，Gd，Tb，Dy，Ho，Er，Tm，Yb和Lu）都是电子中性分子簇，不溶于水和常见的有机溶剂。已经通过实验和计算方法研究了它们的电子结构，电化学性质和催化活性。特别地，基于温和且可控的合成方法，已经开发了一种方便且可控的方法来制备这些单体的纳米晶体和自组织的聚集体。它们对氰基硅烷化显示出显着的非均相催化活性。理论计算表明，标题化合物中RE的Lewis酸强度增加，而粒径减小则有助于其高催化性能。
更新日期：2018-05-11
中文翻译：
稀土多金属氧酸盐纳米晶的可控合成及催化性能
稀土多金属氧酸盐（RE-POMs）催化剂的纳米晶体的大规模分离在基础研究和应用中很重要。在这里，我们通过Ta / W混合齿顶POM {P 2 W 15 Ta 3 O 62 }和稀土（RE）离子的自组装合成了一系列单体RE-POM 。这些分子式为[RE（H 2 O）7 ] 3 P 2 W 15 Ta 3 O 62 · n H 2的RE-POMO（RE = Y，Eu，Gd，Tb，Dy，Ho，Er，Tm，Yb和Lu）都是电子中性分子簇，不溶于水和常见的有机溶剂。已经通过实验和计算方法研究了它们的电子结构，电化学性质和催化活性。特别地，基于温和且可控的合成方法，已经开发了一种方便且可控的方法来制备这些单体的纳米晶体和自组织的聚集体。它们对氰基硅烷化显示出显着的非均相催化活性。理论计算表明，标题化合物中RE的Lewis酸强度增加，而粒径减小则有助于其高催化性能。
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