Yang Tian, Yang Juntao, Deng Xin, Franz Evanie, Fromm Lukas, Taccardi Nicola, Liu Zhi, Görling Andreas, Wasserscheid Peter, Brummel Olaf, Libuda Jörg
Interface Research and Catalysis, FAU Erlangen-Nürnberg, Germany.
School of Physical Science and Technology, Shanghai Tech University, China.
Angew Chem Int Ed Engl. 2022 Jul 18;61(29):e202202957. doi: 10.1002/anie.202202957. Epub 2022 May 24.
The "solid catalyst with ionic liquid layer" (SCILL) is an extremely successful new concept in heterogeneous catalysis. The idea is to boost the selectivity of a catalyst by its modification with an ionic liquid (IL). Here, we show that it is possible to use the same concept in electrocatalysis for the selective transformation of organic compounds. We scrutinize the electrooxidation of 2,3-butanediol, a reaction which yields two products, singly oxidized acetoin and doubly oxidized diacetyl. When adding the IL (1-ethyl-3-methyl-imidazolium trifluormethanesulfonate, [C C Im][OTf]), the selectivity for acetoin increases drastically. By in situ spectroscopy, we analyze the underlying mechanism: Specific adsorption of the IL anions suppresses the activation of water for the second oxidation step and, thus, enhances the selectivity for acetoin. Our study demonstrates the great potential of this approach for selective transformation of organic compounds.
“离子液体层固体催化剂”（SCILL）是多相催化领域一个极其成功的新概念。其理念是通过用离子液体（IL）对催化剂进行改性来提高催化剂的选择性。在此，我们表明可以在电催化中运用相同概念实现有机化合物的选择性转化。我们详细研究了2,3 - 丁二醇的电氧化反应，该反应会产生两种产物，单氧化的乙偶姻和双氧化的二乙酰。当加入离子液体（1 - 乙基 - 3 - 甲基 - 咪唑三氟甲磺酸盐，[C C Im][OTf]）时，对乙偶姻的选择性大幅提高。通过原位光谱分析，我们剖析了其潜在机制：离子液体阴离子的特异性吸附抑制了水在第二步氧化中的活化，从而提高了对乙偶姻的选择性。我们的研究证明了这种方法在有机化合物选择性转化方面的巨大潜力。
