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Title: Ionic Liquid-Stabilized Single-Atom Rh Catalyst against Leaching
Authors: Ding, S 
Hülsey, MJ 
An, H
He, Q 
Asakura, H
Gao, M
Hasegawa, JY
Tanaka, T
Yan, N 
Issue Date: 1-Oct-2021
Publisher: Chinese Chemical Society
Citation: Ding, S, Hülsey, MJ, An, H, He, Q, Asakura, H, Gao, M, Hasegawa, JY, Tanaka, T, Yan, N (2021-10-01). Ionic Liquid-Stabilized Single-Atom Rh Catalyst against Leaching. CCS Chemistry 3 (10) : 1814-1822. ScholarBank@NUS Repository.
Abstract: Single-atom catalysts (SACs) are promising in some reactions typically promoted by homogeneous catalysts. However, the leaching of active species from the support in liquid-phase reactions hinders their potential applications. Herein, taking the hydroformylation reaction as an example, we report ionic liquid (IL)-induced stabilization of single Rh atoms against leaching. Among the ILs examined, 1-(2-hydroxyethyl)-3-methylimidazolium bis(trifluoromethanesulfonyl)imide ([OHEmim][Tf2N])-stabilized single-atom Rh1/TiO2 showed a turnover frequency (TOF) of around 800 h−1 in styrene hydroformylation and was able to be recycled for five runs without significant deactivation. At the same time, the activity for unprotected Rh1/TiO2 decreased over two orders of magnitude under similar conditions. Density-functional theory (DFT) simulations revealed that the IL acts as a linker to connect both Rh and TiO2, thereby enhancing the binding energy of Rh species on TiO2 from 0.69 to 1.19 eV. This work offers a new approach to enhance the stability of atomically dispersed metal catalysts against leaching.
Source Title: CCS Chemistry
ISSN: 20965745
DOI: 10.31635/ccschem.021.202101063
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