期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 141, 期 37, 页码 14772-14779出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b06824
关键词
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资金
- CNRS
- University of Poitiers
- Region Nouvelle Aquitaine
- International Consortium on Ecoconception and Renewable Resources [FR CNRS INCREASE 3707]
- National Research Foundation (NRF)
- Prime Minister's Office
- Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) program
We report here, and rationalize, a synergistic effect between a non-noble metal oxide catalyst (CuO) and high-frequency ultrasound (HFUS) on glucose oxidation. While CuO and HFUS are able to independently oxidize glucose to gluconic acid, the combination of CuO with HFUS led to a dramatic change of the reaction selectivity, with glucuronic acid being formed as the major product. By means of density functional theory (DFT) calculations, we show that, under ultrasonic irradiation of water at 550 kHz, the surface lattice oxygen of a CuO catalyst traps IA- radicals stemming from the sonolysis of water, making the ring-opening of glucose energetically unfavorable and leaving a high coverage of center dot OH radical on the CuO surface, which selectively oxidizes glucose to glucuronic acid. This work also points toward a path to optimize the size of the catalyst particle for an ultrasonic frequency that minimizes the damage to the catalyst, resulting in its successful reuse.
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