In
this work, a hollow double-shelled architecture, based on n-type
ZnIn2S4 nanosheet-coated p-type CuS hollow octahedra
(CuS@ZnIn2S4 HDSOs), is designed and fabricated
as a p–n heterojunction photocatalyst for selective CO2 photoreduction into CH4. The resulting hybrids
provide rich active sites and effective charge migration/separation
to drive CO2 photoreduction, and meanwhile, CO detachment
is delayed to increase the possibility of eight-electron reactions
for CH4 production. As expected, the optimized CuS@ZnIn2S4 HDSOs manifest a CH4 yield of 28.0
μmol g–1 h–1 and a boosted
CH4 selectivity up to 94.5%. The decorated C60 both possesses high electron affinity and improves catalyst stability
and CO2 adsorption ability. Thus, the C60-decorated
CuS@ZnIn2S4 HDSOs exhibit the highest CH4 evolution rate of 43.6 μmol g–1 h–1 and 96.5% selectivity. This work provides a rational
strategy for designing and fabricating efficient heteroarchitectures
for CO2 photoreduction.
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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