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Dynamic Cu(I)/Cu(II) Redox Shuttle for Maltose and Lactose Isomerization under Pulsed Electric Field
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2024-04-09 , DOI: 10.1021/acssuschemeng.3c08073 Ruixuan Zhao 1 , Hongguang Zhang 2 , Renjie Zhao 1 , Wei Liu 1 , Qiannan Liu 1 , Honghai Hu 1
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2024-04-09 , DOI: 10.1021/acssuschemeng.3c08073 Ruixuan Zhao 1 , Hongguang Zhang 2 , Renjie Zhao 1 , Wei Liu 1 , Qiannan Liu 1 , Honghai Hu 1
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Due to their prebiotic effects, lactulose and maltulose have garnered increasing interest from the food and pharmaceutical industries. Pulsed electric field (PEF) technology can enhance energy use efficiency, particularly in electroactivation, offering a potential means to convert reducing sugars. A specialized PEF-treated design has been developed to facilitate alternative catalyst-driven production of lactulose and maltulose by manipulating the morphology and oxidation states of copper catalysts. Under optimal conditions (4 kV/cm, 50 Hz, and 10 μs for 30 min), remarkable yields of lactulose (55.75%) and maltulose (43.27%) were achieved. Higher conversion rates were observed with an increased PEF treatment electric field strength and pulse width. The yields and selectivities of lactulose and maltulose were not significantly influenced by the frequency. Intriguingly, structural monosaccharides, including glucose, galactose, xylose, and arabinose, were also detected in the isomerization reaction. These findings suggest that PEF, utilizing CuO plates, induces glycoside bond hydrolysis and the conversion of aldose to pentose. Microscopic measurements (high-resolution transmission electron microscopy (HRTEM), high-energy X-ray diffraction (XRD), in situ Raman, and X-ray photoelectron spectroscopy (XPS)) revealed that transient Lewis acid–base pairs formed by the Cu+/Cu2+ shuttle could serve as active sites for reducing sugar isomerization, and DFT simulation further confirmed that the presence of active Cu species could promote the isomerization of lactose and maltose via a lower energy barrier. The PEF process proves to be an economical method for transforming low-value sugars into high-value carbon materials.
中文翻译：
脉冲电场下麦芽糖和乳糖异构化的动态 Cu(I)/Cu(II) 氧化还原穿梭
由于其益生元作用，乳果糖和麦芽糖越来越受到食品和制药行业的关注。脉冲电场（PEF）技术可以提高能源利用效率，特别是在电活化方面，为转化还原糖提供了一种潜在的手段。我们开发了一种专门的 PEF 处理设计，通过操纵铜催化剂的形态和氧化态，促进替代催化剂驱动的乳果糖和麦芽糖生产。在最佳条件下（4 kV/cm，50 Hz，10 μs，30 分钟），乳果糖（55.75%）和麦芽糖（43.27%）的产率达到了显着的水平。随着 PEF 处理电场强度和脉冲宽度的增加，观察到更高的转化率。乳果糖和麦芽糖的产量和选择性不受频率的显着影响。有趣的是，在异构化反应中还检测到了结构单糖，包括葡萄糖、半乳糖、木糖和阿拉伯糖。这些发现表明，PEF 利用 CuO 板诱导糖苷键水解以及醛糖转化为戊糖。显微测量（高分辨率透射电子显微镜（HRTEM）、高能 X 射线衍射（XRD）、原位拉曼和 X 射线光电子能谱（XPS））表明，Cu 形成的瞬态路易斯酸碱对+ /Cu 2+穿梭可以作为还原糖异构化的活性位点，DFT模拟进一步证实活性Cu物种的存在可以通过较低的能垒促进乳糖和麦芽糖的异构化。 PEF工艺被证明是将低价值糖转化为高价值碳材料的经济方法。
更新日期：2024-04-09
中文翻译：
脉冲电场下麦芽糖和乳糖异构化的动态 Cu(I)/Cu(II) 氧化还原穿梭
由于其益生元作用，乳果糖和麦芽糖越来越受到食品和制药行业的关注。脉冲电场（PEF）技术可以提高能源利用效率，特别是在电活化方面，为转化还原糖提供了一种潜在的手段。我们开发了一种专门的 PEF 处理设计，通过操纵铜催化剂的形态和氧化态，促进替代催化剂驱动的乳果糖和麦芽糖生产。在最佳条件下（4 kV/cm，50 Hz，10 μs，30 分钟），乳果糖（55.75%）和麦芽糖（43.27%）的产率达到了显着的水平。随着 PEF 处理电场强度和脉冲宽度的增加，观察到更高的转化率。乳果糖和麦芽糖的产量和选择性不受频率的显着影响。有趣的是，在异构化反应中还检测到了结构单糖，包括葡萄糖、半乳糖、木糖和阿拉伯糖。这些发现表明，PEF 利用 CuO 板诱导糖苷键水解以及醛糖转化为戊糖。显微测量（高分辨率透射电子显微镜（HRTEM）、高能 X 射线衍射（XRD）、原位拉曼和 X 射线光电子能谱（XPS））表明，Cu 形成的瞬态路易斯酸碱对+ /Cu 2+穿梭可以作为还原糖异构化的活性位点，DFT模拟进一步证实活性Cu物种的存在可以通过较低的能垒促进乳糖和麦芽糖的异构化。 PEF工艺被证明是将低价值糖转化为高价值碳材料的经济方法。
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