Selectivity Control in the Oxidative Ring-Opening of Dimethylfuran Mediated by Zeolitic-Imidazolate Framework-8 Nanoparticles,ACS Sustainable Chemistry & Engineering

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Selectivity Control in the Oxidative Ring-Opening of Dimethylfuran Mediated by Zeolitic-Imidazolate Framework-8 Nanoparticles
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-06-10 , DOI: 10.1021/acssuschemeng.1c00708
Ana Franco ₁ , Arvind Negi _{1,

2} , Rafael Luque _{1,

3} , Carolina Carrillo-Carrión ₁

Affiliation

The conversion of biomass-derived furans to synthetically valuable chemicals is highly desirable but it remains a formidable challenge with regard to product selectivity, particularly in oxidative reactions. For example, the oxidative ring-opening of 2,5-dimethylfuran (DMF) using hydrogen peroxide as the oxidant proceeds in a nonselective manner, resulting in a multicomponent mixture along with the target compound (3-hexene-2,5-dione). In this work, we address the selectivity issue with a simple and efficient approach using zeolitic-imidazolate framework-8 nanoparticles (ZIF-8 NPs) as selectivity mediators on the base of their unique ordered structure. A quantitative conversion of DMF with 85% of selectivity to the target 3-hexene-2,5-dione (in comparison to 27% selectivity in the blank reaction) was achieved in the presence of ZIF-8 NPs, and importantly, under mild conditions (60 °C, and methanol as solvent). Furthermore, computational studies based on the chemisorption models of ZIF-8 demonstrated a plausible explanation of the observed selectivity. This work may pave the way toward the development of alternative and cost-effective strategies to improve product selectivity in biomass conversion with a view of green and sustainable developments in the chemical industry.

中文翻译：

沸石-咪唑酯骨架-8纳米颗粒介导的二甲基呋喃氧化开环的选择性控制

将生物质衍生的呋喃转化为具有合成价值的化学品是非常可取的，但在产品选择性方面，尤其是在氧化反应中，这仍然是一项艰巨的挑战。例如，使用过氧化氢作为氧化剂的 2,5-二甲基呋喃 (DMF) 的氧化开环以非选择性方式进行，导致多组分混合物与目标化合物 (3-己烯-2,5-二酮) . 在这项工作中，我们使用沸石-咪唑酯骨架-8 纳米颗粒（ZIF-8 NPs）基于其独特的有序结构作为选择性介质，通过一种简单有效的方法解决了选择性问题。在 ZIF-8 NP 存在下，DMF 以 85% 的选择性转化为目标 3-己烯-2,5-二酮（相比之下，空白反应的选择性为 27%），重要的是，在温和条件下（60 °C，甲醇为溶剂）。此外，基于 ZIF-8 化学吸附模型的计算研究证明了对观察到的选择性的合理解释。从化学工业的绿色和可持续发展的角度来看，这项工作可能为开发替代和具有成本效益的策略铺平道路，以提高生物质转化中的产品选择性。

更新日期：2021-06-21

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