Photocatalytic
CO2 reduction is hampered by the inefficient
charge separation and kinetically challenging interfacial reaction.
Combining nonprecious cocatalysts with semiconductors is vital for
optimizing these processes. Herein, a step-by-step route is reported
for the in situ growth of island-shaped graphene on TaON particles
(TaON@G) with controllable distribution, targeting a superior photocatalyst
for visible-light-driven CO2 reduction. The TaON@G photocatalyst
possesses the snug contact interface with suitable interfacial energy
levels for accelerating the charge separation, the island-shaped graphene
with a hollow nanoarchitecture for facilitating the adsorption of
CO2, and the hierarchical structure with spatially separated
active sites for activating CO2 and promoting proton release.
The optimized TaON@G achieves a visible-light-driven CO2-to-CH4 yield of 1.61 μmol g–1 h–1, which is nearly 13-fold higher compared with
that of pristine TaON and outperforms most Ta-based (oxy)nitride catalysts.
Density functional theory calculations further elucidate the enhanced
activity, suggesting that TaON interacts with graphene strongly with
the charge transfer from TaON to graphene, inducing electron-rich
graphene with a significant upshift of the graphene Fermi level, leading
to a high filling fraction of the antibonding orbitals, thereby weakening
the CO bond of the adsorbed CO2 for breaking. Our
study highlights the importance of rational design of well-defined
hierarchical photocatalysis to synergistically integrate the structural
and functional advantages for maximizing catalytic performance.
Solar‐driven CO2 conversion to fuels is a central technique for closing the anthropogenic carbon cycle, but to date is limited by the intermittent solar flux. To face this challenge, a catalyst is needed that can work well in both light and dark. Here, surface oxygen vacancies are created in a Sr2MgSi2O7:Eu2+,Dy3+ long‐afterglow phosphor with long‐time and high charge storage capacity (denoted as Vo‐SMSED) as both electron transfer station and active sites for molecule activation. The strong ability for oxygen vacancies to store and extract electrons from charge storage centers enables the Vo‐SMSED to work efficiently in both light and dark. As a result, Vo‐SMSED manifests nearly 100% selectivity for catalyzing CO2 reduction by H2O to CO with high light stability and over 3 h dark activity. These results demonstrate that creating the bifunctional sites as electron‐storing/extracting and molecule‐activating center is an efficient route to change the long‐lived charge into the highly active species for catalysis, thus making the long‐afterglow phosphors with high charge storage capacity a highly efficient round‐the‐clock photocatalyst.
Z-scheme system was successfully constructed for visible light driven photocatalytic H2 production from lignocelluloses, the highest H2 evolution rate of this Z-scheme system achieves 5.3 and 1.6 μmol•h-1 in α-celluloses...
Benefiting from their structural and compositional merits, the as-synthesized CoP@Ni2P core–shell nanoarrays exhibit excellent electrocatalytic activity and long-term stability for HER in 1 M KOH.
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