Sun Q,
Wang N,
Zhang T,
Bai R,
Mayoral A.
*
Zhang P,
Zhang Q,
Terasaki O,
Yu J.
* ShanghaiTech University and Jilin University, Changchun, P. R. of China
Zeolite-Encaged Single-Atom Rhodium Catalysts: Highly-Efficient Hydrogen Generation
and Shape-Selective Tandem Hydrogenation of Nitroarenes.
Angew. Chem. Int. Ed. 2019;
58: 18570-18576
Key words
rhodium catalysis - reduction - nitroarenes - ammonia–borane - anilines
Significance
A single-atom rhodium catalyst immobilized on silicate-1 zeolite (Rh@S-1-H), prepared
as shown in equation 1, catalyzed the hydrolysis of ammonia–borane with a turnover
frequency of 432 molH2 molRh
–1 min–1 (eq. 2). A sequential hydrolysis of ammonia–borane and hydrogenation of nitroarenes
also proceeded in the presence of Rh@S-1-H (eq. 3).
Comment
As shown in equation 3, p-substituted nitrobenzenes were reduced to the corresponding anilines with 100% conversion
and >99% selectivity, whereas m-substituted nitrobenzenes were almost intact after the hydrogenation reaction. Rh@S-1-H
was characterized by means of 13C MAS-NMR, TG-DTA, PXRD, ICP-AES, HAADF-STEM, HRTEM, SEM, EDS, XPS, XANES, EXAFS,
and CO-DRIFTS measurements.
