Exploring
cheap and efficient hybrid catalysts offers exciting
opportunities for enhancing the performance of photocatalysts in the
green organic synthesis field. Herein, a facile and effective approach
is designed for the synthesis of a sandwich-structured hybrid in which
NiCo bimetallic nanoparticles are embedded in the tip of nitrogen-doped
carbon nanotubes (N-CNTs) grafted on both sides of a nitrogen deficient
C3N4 (Nv-C3N4) nanosheet for photodehydrogenative coupling reactions. Such a brand-new
type of sandwich-structured hybrid comprises Nv-C3N4 nanosheets and surrounding N-CNTs embedded with NiCo
nanoparticles at their tips. Remarkably, the resultant hybrid exhibits
integrated functionalities, abundant active sites, enhanced visible
light absorption, and excellent interfacial charge transfer ability.
As a result, the optimized NiCo@N-CNTs@Nv-C3N4 photocatalyst shows significantly improved photodehydrogenative
coupling performance of amines to imines compared to the control single-metal-based
catalysts (Ni@N-CNTs@Nv-C3N4 and
Co@N-CNTs@Nv-C3N4). The mechanistic
investigation through experimental and computational study demonstrates
that, compared with single-metal-based hybrids, the NiCo bimetallic
hybrid exhibits stronger amine adsorption and weaker photogenerated
hydrogen atom adsorption, thus promoting the dehydrogenative activation
of primary amines and fast generation of imines. This work presents
a promising insight for designing and preparing efficient photocatalysts
to trigger organic synthesis in high yields.
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