Single-atom catalysts (SACs) have attracted considerable attention in the catalysis community. However, fabricating intrinsically stable SACs on traditional supports (N-doped carbon, metal oxides, etc.) remains a formidable challenge, especially under hightemperature conditions. Here, we report a novel entropy-driven strategy to stabilize Pd single-atom on the high-entropy fluorite oxides (CeZrHfTiLa)O x (HEFO) as the support by a combination of mechanical milling with calcination at 900°C. Characterization results reveal that single Pd atoms are incorporated into HEFO (Pd 1 @HEFO) sublattice by forming stable Pd-O-M bonds (M = Ce/Zr/La). Compared to the traditional support stabilized catalysts such as Pd@CeO 2 , Pd 1 @HEFO affords the improved reducibility of lattice oxygen and the existence of stable Pd-O-M species, thus exhibiting not only higher low-temperature CO oxidation activity but also outstanding resistance to thermal and hydrothermal degradation. This work therefore exemplifies the superiority of high-entropy materials for the preparation of SACs.
Photocatalytic
CO2 reduction to solar fuel is a promising
route to alleviate the ever-growing energy crisis and global warming.
Herein, to enhance photoconversion efficiency of CO2 reduction,
a series of direct Z-scheme composites consisting of β-AgVO3 nanoribbons and InVO4 nanoparticles (InVO4/β-AgVO3) are prepared via a facile hydrothermal
method and subsequent in situ growth process. The prepared InVO4/β-AgVO3 composites exhibit enhanced photocatalytic
activity for reduction of CO2 to CO under visible-light
illumination. A CO evolution rate of 12.61 μmol·g–1·h–1 is achieved over the optimized 20% In–Ag
without any cocatalyst or sacrificial agent, which is 11 times larger
than that yielded by pure InVO4 (1.12 μmol·g–1·h–1). Moreover, the CO selectivity
is more than 93% over H2 production from the side reaction
of H2O reduction. Significantly, based on the results of
electron spin resonance (ESR) and in situ irradiated XPS tests, it
is proposed that the synthesized InVO4/β-AgVO3 catalysts comply with the direct Z-scheme transfer mechanism.
Significantly improved photocatalytic activities for selective CO2 reduction could be primarily ascribed to effective separation
of photoinduced electron–hole pairs and enhanced reducibility
of photoelectrons at the conduction band of InVO4. This
work provides a new insight for constructing highly efficient photocatalytic
CO2 reduction systems toward solar fuel generation.
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