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.
NH3 emissions were limited strictly because of the threat for human health and sustainable development. Pt/Al2O3 and Pt/CeZrO2 were prepared by the impregnation method. Differences in surface chemical states, reduction ability, acid properties, morphological properties, reaction mechanisms, and ammonia oxidation activity were studied. It indicated that Pt species states were affected by different metal–support interactions. The homogeneously dispersed Pt species over Pt/Al2O3 exposed Pt(111) because of weak metal–support interactions; there even existed an obvious interface between Pt and Al2O3. While obscure even an overlapped interface was observed over Pt/CeZrO2, resulting in the formation of PtO because of the oxygen migration from CeZrO2 to Pt species (confirmed by CO-FTIR, the cycled H2-TPR and transmission electron microscopy results). It was noteworthy that different reaction mechanisms were induced by different states of Pt species; NH was the key intermediate species for ammonia oxidation reaction over Pt/Al2O3, but two kinds of intermediates, N2H4 and HNO, were observed for Pt/CeZrO2. It consequently resulted in the obvious distinction of the NH3-SCO catalytic performance; the light-off temperatures of NH3 over Pt/Al2O3 and Pt/CeZrO2 were 231 and 275 °C, respectively, while the maximum N2 selectivity (65%) was obtained over Pt/CeZrO2, it was obviously better than that over Pt/Al2O3.
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