POM-FLPs: [MoIV 3 ]n-polyoxometalate bifunctional catalysis by [MoIV 3 ]n–Om Lewis pairs frustrated by triangular MoIV–MoIV bonds

POM-FLPs: [MoIV 3 ]n-polyoxometalate bifunctional catalysis by [MoIV 3 ]n–Om Lewis pairs frustrated by triangular MoIV–MoIV bonds
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POM-FLP:[MoIV 3 ]n-多金属氧酸盐双功能催化[MoIV 3 ]n-Om路易斯对被三角形MoIV-MoIV键抑制

DOI:
10.1039/c9dt00983c
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发表时间:
2019
影响因子:
4
通讯作者:
Li Xu
Li Xu
中科院分区:
化学2区
文献类型:
--
作者:
Benlong Luo;Li Xu

文献摘要

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路易斯酸和路易斯碱基对结合在一个单一的体系中是新兴的。双功能催化的活跃前沿领域。作为高效的刘易斯酸和刘易斯碱双功能催化剂,更能还原MoIV。具有多个MoIV - (μ2-O)路易斯对的n -多金属氧酸盐。是必要的。将新型混合溶剂吡啶/DMF/H2O和异金属氧化物(GeO2)引入到[Mo3O2(O2CCH3)6(H2O)3]ZnCl4的溶剂热部分氧化体系中,得到了收率。2 .小说[电影][3]n-POM家族成员,H4[Mo@MoIV.6]O54(OH)4py6] ({Mo@Mo20}-1)和.[Ge@MoIV.6 MoVI.10Zn0.5Ge1.5O47.5(H2O)0.5py6] ({Ge@Mo16Ge1.5Zn0.5}-2),提供了两条新的重要路线。扩展POM-FLP系统,并允许系统地研究它们的合理合成。不同的分子和电子结构及其对催化效率的影响。POM-FLP。该体系具有优异的选择性(>97%)和结构依赖的转化。HOMO MoIV百分比,[MoIV]的数量和连锁。[3]n - (μ2-O)m FLPs在联氨转移中的作用。硝基苯加氢还原为苯胺,有利于达到最佳的催化性能。POM-FLP体系在转移加氢或其他催化反应中的应用。
Lewis acid and Lewis base pairs combined in a single system are emerging as one of the most.active frontier areas in bifunctional catalysis. To serve as efficient Lewis acid and Lewis base bifunctional.catalysts, more reduced MoIV.n -polyoxometalates having multiple MoIV–(μ2-O) Lewis pairs.are necessary. The new mixed solvent pyridine/DMF/H2O and heterometal oxide (GeO2) have been.introduced into the solvothermal partial oxidation system of [Mo3O2(O2CCH3)6(H2O)3]ZnCl4 to yield.two novel [MoIV.3 ]n-POM family members, H4[Mo@MoIV.6 MoV6.MoVI.8 O54(OH)4py6] ({Mo@Mo20}-1) and.[Ge@MoIV.6 MoVI.10Zn0.5Ge1.5O47.5(H2O)0.5py6] ({Ge@Mo16Ge1.5Zn0.5}-2), providing two new important routes.to extend the POM-FLP system and allowing for a systematic investigation into their reasonable syntheses,.diverse molecular and electronic structures, and their influence on the catalytic efficiency. The POM-FLP.system exhibits excellent selectivity (>97%) and structure-dependent conversion dominated by the.HOMO MoIV percentage, and the number and linkage of [MoIV.3 ]n–(μ2-O)m FLPs in the hydrazine transfer.hydrogenation reduction of nitrobenzene to aniline, which is helpful to achieve optimal catalysis performance.of the POM-FLP system in transfer hydrogenation or other catalysis reactions that are yet to be.developed.