Rational Design of a Polyoxometalate Intercalated Layered Double Hydroxide: Highly Efficient Catalytic Epoxidation of Allylic Alcohols under Mild and Solvent-Free Conditions

Tengfei Li; Zelin Wang; Wei Chen; Haralampos N. Miras; Yu-Fei Song

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Rational Design of a Polyoxometalate Intercalated Layered Double Hydroxide: Highly Efficient Catalytic Epoxidation of Allylic Alcohols under Mild and Solvent-Free Conditions

机译：多氧化素嵌入层双氢氧化物的合理设计：轻度和无溶剂条件下烯丙基醇的高效催化环氧化

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Intercalation catalysts, owing to their modular and accessible gallery and unique interlamellar chemical environment, have shown wide application in various catalytic reactions. However, the poor mass transfer between the active components of the intercalated catalysts and organic substrates is one of the challenges that limit their further application. Herein, we have developed a novel heterogeneous catalyst by intercalating the polyoxometalate (POM) of Na_9LaW_(10)O_(36)·32H_2O (LaW_(10)) into layered double hydroxides (LDHs), which have been covalently modified with ionic liquids (ILs). The intercalation catalyst demonstrates high activity and selectivity for the epoxidation of various allylic alcohols in the presence of H_2O_2. For example, trans-2-hexen-1-ol undergoes up to 96% conversion and 99% epoxide selectivity at 25°C in 2.5 h. To the best of our knowledge, the Mg_3Al-ILs-C_8-LaW_(10) composite material constitutes one of the most efficient heterogeneous catalysts for the epoxidation of allylic alcohols (including the hydrophobic allylic alcohols with long alkyl chains) reported so far.

机译：由于它们的模块化和可访问的图库并且独特的层间化学环境，嵌入催化剂已经显示出各种催化反应的广泛应用。然而，插层催化剂和有机基材的活性组分之间的差的质量转移是限制其进一步应用的挑战之一。在此，通过将Na_9LAW_（10）O_（36）·32H_2O（LAW_（10））的聚氧酸盐（POM）相邻，开发了一种新型的异构催化剂，进入层状的双氢氧化物（LDH），该双氢氧化物（LDHS）将其与离子液体共价改性（ ILS）。嵌入催化剂在H_2O_2的存在下，表现出各种烯丙基醇的环氧化的高活性和选择性。例如，Trans-2-Hexen-1-OL在2.5小时内在25℃下进行高达96％的转化率和99％环氧化物选择性。据我们所知，Mg_3Al-ILS-C_8-LAM_（10）复合材料构成到目前为止所报告的烯丙基醇环氧化的最有效的异质催化剂之一。

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来源
《Chemistry: A European journal》 |2017年第5期|共9页
作者
Tengfei Li; Zelin Wang; Wei Chen; Haralampos N. Miras; Yu-Fei Song;
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作者单位

State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing 100029 (P.R. China);

State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing 100029 (P.R. China);

State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing 100029 (P.R. China);

WestCHEM School of Chemistry University of Glasgow Glasgow G12 8QQ (UK);

State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing 100029 (P.R. China);

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原文格式 PDF
正文语种 eng
中图分类应用化学;
关键词
allylic compounds; epoxidation; ionic liquids; layered compounds; polyoxometalates;

机译：烯丙基化合物;环氧化;离子液体;层状化合物;聚毒液酸盐;

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1. Rational Design of a Polyoxometalate Intercalated Layered Double Hydroxide: Highly Efficient Catalytic Epoxidation of Allylic Alcohols under Mild and Solvent-Free Conditions [J] . Tengfei Li, Zelin Wang, Wei Chen, Chemistry: A European journal . 2017,第5期

机译：多氧化素嵌入层双氢氧化物的合理设计：轻度和无溶剂条件下烯丙基醇的高效催化环氧化
2. Highly Efficient Catalytic Asymmetric Epoxidation of Allylic Alcohols by an Oxovanadium-Substituted Polyoxometalate with a Regenerative TADDOL-Derived Hydroperoxide [J] . Waldemar Adam, Paul L. Alsters, Ronny Neumann, Organic letters . 2003,第5期

机译：氧代钒取代多金属氧酸盐与可再生TADDOL衍生的过氧化氢对烯丙醇的高效催化不对称环氧化
3. The application of spontaneous flocculation for the preparation of lanthanide-containing polyoxometalates intercalated layered double hydroxides: highly efficient heterogeneous catalysts for cyanosilylation [J] . Yueqingjia, Shen Zhao, Yu-Fei Song Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications . 2014,第Null期

机译：自发絮凝在制备含镧系元素多金属氧酸盐插层双氢氧化物中的应用：氰基硅烷化反应的高效多相催化剂
4. Intercalated Layered Double Hydroxides M~(2+)/M~(3+) (M~(2+): Mg, Ca, Ni; M~(3+): Al) with Tungstosilicate Polyoxometalate [C] . A. Lesbani, T. Taher, N. R. Palapa, International Symposium on Current Progress in Mathematics and Sciences . 2020

机译：嵌入层状双氢氧化物M〜（2 +）/ m〜（3+）（M〜（2+）：mg，Ca，Ni; m〜（3+）：Al）用钨硅酸盐聚毒液酸盐
5. Layered double hydroxides: I. Synthesis by design. II. Catalysis by intercalated polyoxometalates. [D] . Gardner, Elizabeth Ann. 1998

机译：层状双氢氧化物：I.设计合成。二。插层多金属氧酸盐的催化作用。
6. Highly Efficient Lithium Recovery from Pre-Synthesized Chlorine-Ion-Intercalated LiAl-Layered Double Hydroxides via a Mild Solution Chemistry Process [O] . Ying Sun, Rongping Yun, Yufeng Zang, 2019

机译：通过温和的溶液化学过程从预合成的氯离子嵌入的LiAl层状双氢氧化物中高效回收锂
7. Rational design of a polyoxometalate intercalated layered double hydroxide: highly efficient catalytic epoxidation of allylic alcohols under mild and solvent-free conditions [O] . Li Tengfei, Wang Zelin, Chen Wei, 2017

机译：多金属氧酸盐嵌入层状双氢氧化物的合理设计：在温和无溶剂条件下高效催化环氧化烯丙醇

Rational Design of a Polyoxometalate Intercalated Layered Double Hydroxide: Highly Efficient Catalytic Epoxidation of Allylic Alcohols under Mild and Solvent-Free Conditions

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