.png){kind=icon}
.png){kind=icon}
Return
C-N bond formation from co-conversion of N2 and CO2 mediated by Nb2OH4- cluster anions: importance of hydride ligands
.png){kind=icon}
PRE
AI
L
L
Z
S
DOI：10.1039/d6cp00218h.png)
.png){kind=icon}
Original request for help.png){kind=icon}
Share.png){kind=icon}
Save
Abstract
En 中文
Constructing C-N bonds directly from N2 and CO2 is highly desirable but challenging. Although metal hydrides show promise in N2 activation and functionalization with CO2, their precise role in selectively facilitating C-N coupling remains unclear. Herein, we report the C-N bond formation in the co-conversion of N2 and CO2 mediated by a dinuclear metal hydride cluster Nb2OH4- employing mass spectrometry and quantum chemistry calculations. The key intermediate Nb2OH2N2-, derived from the preliminary reaction of Nb2OH4- with N2, could react with CO2 to form the C-N bond, as evidenced by the detection of fragment ions (NC- and NCO-). Mechanistic studies indicate that hydride ligands modulate the electronic structure of metal centers by weakening the reducing ability and enabling moderated CO2 activation that favors C-N coupling over CO2 reduction. The work elucidates how the formation of well-controlled metal hydrides governs electronic structure and reaction pathways, establishing a general design principle for achieving selective N2-CO2 coupling and direct C-N bond construction.
Keywords:
CARBON-DIOXIDE ACTIVATION
DINITROGEN
HYDROGENATION
Journal
IF:
2.9
Papers:
4.3K
Citations:
12.4W
Organization
Cited Papers