Molten salt-induction of geometrically deformed ruthenium single atom catalysts with high performance for aerobic oxidation of alcohols

• Published in: Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2023-01, Vol.451, p.138660, Article 138660
• Main Authors: Dong, Xiuli, Jia, Yufei, Zhang, Mingyang, Ji, Siqi, Leng, Leipeng, Hugh Horton, J., Xu, Chang, He, Cheng, Tan, Qiang, Zhang, Jiangwei, Li, Zhijun
• Format: Article
• Language: English
• Subjects: Aerobic oxidation of alcohols; Catalytic activity; Nitrogen-doped carbon; Ruthenium; Single atom catalysis
• ISSN: 1385-8947; 1873-3212
• DOI: 10.1016/j.cej.2022.138660

[Display omitted] •Molten salt-induced geometrically deformed Ru single atom catalyst was created.•DFT calculations reveal the NC support can provide anchoring sites for Ru atoms.•This catalyst shows high catalytic efficacy in the aerobic oxidation of alcohols.•The high catalytic activity stems from electronic metal-support interactions. Recently, construction of single atom catalysts (SACs) for heterogeneous organic transformations has attracted great interest, but accomplishing high selectivity for a specific product under mild conditions remains challenging. Herein, we report a facile molten salt-induced strategy for creating Ru single atoms anchored onto a geometrically deformed nitrogen-doped carbon (Ru1/NC) support. This Ru catalyst is characterized by a range of methods, including advanced electron microscopy and X-ray absorption spectroscopy. The results show that the Ru single atom catalyst is highly effective for benzyl alcohol oxidation reaction, achieving an exceptional catalytic efficiency (1 atm O2 @ 90 °C) with more than 99 % selectivity for benzaldehyde under nearly 100 % conversion, along with a high initial turnover frequency up to 1213 h−1. Moreover, excellent recyclability and substrate tolerance ability are validated. Density functional theory calculations further indicate that the high catalytic reactivity stems from strong electronic metal-support interactions. This work provides a new avenue in designing single atom catalysts at the atomic level for organic transformations.