瑞士苏黎世大学S. David Tilley团队利用主客体相互作用将分子催化剂固定在电极表面。 相关研究成果发表在2021年3月25日出版的国际学术期刊《自然-化学》。

将分子催化剂锚定在电极表面可以将分子体系的高选择性和高活性以及多相体系的实用性结合在一起。然而，分子催化剂远不如传统的非均相电催化剂稳定，因此一种容易取代已降解的锚定分子催化剂的方法可以使这种电合成系统更具吸引力。

该文中，研究人员应用非共价“点击”化学方法，通过主客体与表面锚定环糊精的络合作用，将分子电催化剂可逆地结合到电极表面。主客体相互作用非常强，使得电子在电极和客体催化剂之间流动。在有机和水介质中的电合成均在金属氧化物电极上进行，稳定性在小时量级。催化表面可以通过控制客体从主体空腔的释放和新鲜客体的再吸附来回收利用。

附：英文原文

Title: Immobilization of molecular catalysts on electrode surfaces using host–guest interactions

Author: Laurent Svery, Jacek Szczerbiski, Mert Taskin, Isik Tuncay, Fernanda Brandalise Nunes, Chiara Cignarella, Gabriele Tocci, Olivier Blacque, Jrg Osterwalder, Renato Zenobi, Marcella Iannuzzi, S. David Tilley

Issue&Volume: 2021-03-25

Abstract: Anchoring molecular catalysts on electrode surfaces combines the high selectivity and activity of molecular systems with the practicality of heterogeneous systems. Molecular catalysts, however, are far less stable than traditional heterogeneous electrocatalysts, and therefore a method to easily replace anchored molecular catalysts that have degraded could make such electrosynthetic systems more attractive. Here we applied a non-covalent ‘click’ chemistry approach to reversibly bind molecular electrocatalysts to electrode surfaces through host–guest complexation with surface-anchored cyclodextrins. The host–guest interaction is remarkably strong and enables the flow of electrons between the electrode and the guest catalyst. Electrosynthesis in both organic and aqueous media was demonstrated on metal oxide electrodes, with stability on the order of hours. The catalytic surfaces can be recycled by controlled release of the guest from the host cavities and the readsorption of fresh guest.

DOI: 10.1038/s41557-021-00652-y

Source: https://www.nature.com/articles/s41557-021-00652-y