期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 14, 期 48, 页码 10832-10846出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.3c02740
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A new microwave route has been developed for the one-pot conversion of pentose and hexose sugars into glycol and hexitol without pressurized hydrogen reactors. The hydrogenolysis of sugars to glycols is achieved using a Ru single atom catalyst on a phosphine-modified silica carrier under mild conditions.
Tandem hydrogenation vis-a-vis hydrogenolysis of xylose to 1,2-glycols remains a major challenge. Although one-pot conversion of xylose to 1,2-glycols requires stringent conditions, a sustainable approach would be quite noteworthy. We have developed a microwave route for the one-pot conversion of pentose (C5) and hexose (C6) sugars into glycol and hexitol, without pressurized hydrogen reactors. A pronounced hydrogenolysis of sugars to glycols is observed by Ru single atom (SA) on triphenylphosphine/phosphine oxide-modified silica (Ru@SiP), in contrast to Ru SA on pristine (Ru@SiC) and 3-aminopropyl-modified silica (Ru@SiN). A promising ligand effect was observed through phosphine modification of silica that presents a 70% overall yield of all reduced sugars (xylitol + glycols) from a 99% conversion of xylose with Ru@SiP. A theoretical study by DFT depicts an electronic effect on Ru-SA by triphenylphosphine that promotes the catalytic hydrogenolysis of sugars under mild conditions. Hence, this research represents an important step for glycols from biomass-derived sources.
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