In:
Angewandte Chemie, Wiley, Vol. 133, No. 43 ( 2021-10-18), p. 23338-23342
Abstract:
One of the most pressing challenges in single‐atom catalysis is the manipulation of the coordination environment of central metals to maximize the catalyst performance. Herein, we fabricated a high‐performance catalyst (Co‐SNC) by introducing S into the neighboring position of the Co‐N 4 coordination. The developed ball‐milling method enabled large‐scale synthesis, that over 4.7 g of Co‐SNC can be produced in one pot. In benzylamine coupling reaction, Co‐SNC exhibited the highest conversion of 97.5 % with 99 % selectivity toward N ‐benzylidenebenzylamine in 10 h among various Co catalysts. Density functional theory calculations revealed the crucial role of S atoms, which serve as the active sites for O 2 activation, leaving the Co atoms free to adsorb benzylamine. Consequently, the adsorption energies of O 2 and benzylamine were significantly increased. Our strategy suggests a feasible approach to enhance catalytic performance by delicately integrating dual active sites into a single catalyst unit.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v133.43
DOI:
10.1002/ange.202109356
Language:
English
Publisher:
Wiley
Publication Date:
2021
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