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首页> 外文期刊>RSC Advances >Cascade catalytic hydrogenation-cyclization of methyl levulinate to form gamma-valerolactone over Ru nanoparticles supported on a sulfonic acidfunctionalized UiO-66 catalyst
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Cascade catalytic hydrogenation-cyclization of methyl levulinate to form gamma-valerolactone over Ru nanoparticles supported on a sulfonic acidfunctionalized UiO-66 catalyst

机译：甲磺酸甲基甲基催化氢化环化在磺酸官能化UIO-66催化剂上负载的Ru纳米粒子上形成γ-戊酮

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摘要

We herein report a high-yielding one-pot upgrade strategy for converting biomass-derived methyl levulinate (ML) into gamma-valerolactone (GVL) over a dual-functional catalyst prepared by depositing Ru nanoparticles on a sulfonic acid-functionalized Zr-based metal-organic framework (SO3H-UiO-66). Under the mild conditions of 80 degrees C and 0.5 MPa H-2 for 4 h in aqueous solution, a quantitative (100%) yield of GVL was obtained over the prepared Ru/SO3H-UiO-66 catalyst. In contrast, a very limited yield of GVL was achieved in the control experiment by first hydrogenating the reactant ML over a metal catalyst without any acidity (e.g. Ru/C) to produce the 4-hydroxypentanoic acid methyl ester (4-HPME) intermediate, followed by treatment of this intermediate over the acidic SO3H-UiO-66 support in the absence of metal. We also found that the catalytic activity and selectivity of Ru/SO3H-UiO-66 were significantly suppressed upon neutralization of its acidic sites, thereby confirming the indispensable role of the sulfonic acid groups in promoting the intramolecular dealcoholation of the 4-HPME intermediate. Furthermore, the Ru/SO3H-UiO-66 catalyst was recyclable over five cycles without any significant loss in its catalytic activity, thus rendering this precious metal/acid dual-functional catalyst a potential candidate for efficient GVL production under mild conditions.
机译：我们在本文中报告了通过在通过在磺酸官能化Zr基金属上沉积Ru纳米粒子制备的双官能催化剂将生物质衍生的甲基乙酰硫酸盐（GV1）转化为γ-戊酰基（GV1）的高产的单罐升级策略 - 无机框架（SO3H-UIO-66）。在水溶液中80℃和0.5MPa H-2的温和条件下，通过制备的Ru / SO 3-UIO-66催化剂获得了GV1的定量（100％）产率。相反，通过在没有任何酸度（例如Ru / C）的金属催化剂上，通过在金属催化剂上氢化反应物M1，在对照实验中实现GV1的非常有限的GV产量，而没有任何酸度（例如RU / C），以制备4-羟基戊烯酸甲酯（4-HPME）中间体，然后在没有金属的情况下处理过酸性SO3H-UIO-66载体的中间体。我们还发现在中和其酸性位点时显着抑制了ru / SO3H-UIO-66的催化活性和选择性，从而证实了磺酸基团在促进4-HPME中间体的分子内脱醇方面的不可缺少作用。此外，Ru / SO3H-UIO-66催化剂在5个循环中可回收，而不在其催化活性中损失任何显着的损失，因此使该贵金属/酸双功能催化剂是在温和条件下有效地产生的潜在候选者。

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  • 来源
    《RSC Advances》 |2017年第70期|共7页
  • 作者

    Lin Zhenzhen; Cai Xiaoxiong; Fu Yanghe; Zhu Weidong; Zhang Fumin;

  • 作者单位

    Zhejiang Normal Univ Inst Adv Fluorine Containing Mat Minist Educ Adv Catalysis Mat Key Lab Jinhua 321004 Peoples R China;

    Zhejiang Normal Univ Inst Adv Fluorine Containing Mat Minist Educ Adv Catalysis Mat Key Lab Jinhua 321004 Peoples R China;

    Zhejiang Normal Univ Inst Adv Fluorine Containing Mat Minist Educ Adv Catalysis Mat Key Lab Jinhua 321004 Peoples R China;

    Zhejiang Normal Univ Inst Adv Fluorine Containing Mat Minist Educ Adv Catalysis Mat Key Lab Jinhua 321004 Peoples R China;

    Zhejiang Normal Univ Inst Adv Fluorine Containing Mat Minist Educ Adv Catalysis Mat Key Lab Jinhua 321004 Peoples R China;

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