Synthesis of Nanosheets Containing Uniformly Dispersed PdII Ions at an Aqueous/Aqueous Interface: Development of a Highly Active Nanosheet Catalyst for Mizoroki-Heck Reaction

Synthesis of Nanosheets Containing Uniformly Dispersed PdII Ions at an Aqueous/Aqueous Interface: Development of a Highly Active Nanosheet Catalyst for Mizoroki-Heck Reaction
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DOI:
10.1021/acsomega.0c02403
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发表时间:
2020-07-28
期刊:
影响因子:
4.1
通讯作者:
Yamanobe, Takeshi
Yamanobe, Takeshi
中科院分区:
化学3区
文献类型:
--
作者:
Nagai, Daisuke;Morita, Moeko;Yamanobe, Takeshi

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开发了一种在 Pd-II 离子水层和带有金属配位单元 (HPMC) 的亲水聚合物水层界面合成纳米片的方法。该纳米片是通过将低比重(1.03 g/cm(3))的Pd-II离子水溶液添加到高比重(1.50 g/cm(3))的HPMC分散水溶液中生成界面,从而在界面处快速交联而合成的。电子探针微量分析图显示 Pd-II 离子均匀分散在纳米片中。该纳米片对Mizoroki-Heck交叉偶联反应表现出较高的催化活性,周转数(TON)和周转频率(TOF)分别大于3,333,333和138,889 h(-1)。这些是 Mizoroki-Heck 反应非均相聚合物催化剂报道的最大 TON 和 TOF 值。
A method was developed to synthesize a nanosheet at the interface of an aqueous layer of Pd-II ions and an aqueous layer of hydrophilic polymer bearing a metal coordination unit (HPMC). The nanosheet was synthesized through generation of an interface by the addition of an aqueous solution of Pd-II ions with a low specific gravity (1.03 g/cm(3)) to a dispersed aqueous solution of HPMC with a high specific gravity (1.50 g/cm(3)), resulting in rapid cross-linkin at the interface. An electron probe microanalysis mapping image showed that the Pd-II ions were uniformly dispersed in the nanosheet. The nanosheet showed a high catalyst activity for the Mizoroki-Heck cross-coupling reaction with a turnover number (TON) and turnover frequency (TOF) greater than 3,333,333 and 138,889 h(-1), respectively. These are the greatest TON and TOF values reported for heterogeneous polymeric catalysts for the Mizoroki-Heck reaction.