Recently, new nanoparticle shaping strategies have been established involving the disassembly of preformed macroscopic architectures by cutting, pasting or merging assembled structures. In prior work 6, three-dimensionally ordered macroporous La 0.6Sr 0.4MnO 3 (3DOM LSMO) was synthesized with a high surface area and a rich presence of surface oxygen species whereby it exhibited a much better catalytic performance than its one-dimensional (1D) counterpart. For example, nanosized particles can significantly increase the surface area and thus increase the contact between reactants and surface active sites 5. It is commonly accepted that scaling down particle dimensions to the nanometre regime can generate unique properties within the material 4. Efforts to minimize the associated activity loss have focused on using perovskite make-up and preparation techniques to influence factors such as element composition, morphology, surface area and structure control. Using a perovskite as a catalyst for methane combustion can improve stability although this is offset by a partial sacrifice in activity. Mixed oxides comprising non-noble metal components seem a more promising alternative, with perovskites having gained particular attention 2, 3. However, the associated high cost and poor thermal stability (caused by agglomeration of the metal deposits) of the catalytic elements persist as major challenges. Precious metals (for example, Pd and Pt) supported on Al 2O 3 are well studied and used as commercial catalysts for complete methane oxidation at low temperatures. Catalytic methane oxidation is often employed to stabilize ‘lean’ flames (those with a low fuel to air ratio) at relatively low temperatures as compared to non-catalytic combustion, thus preventing the formation of noxious nitrogen oxides 1. It is of great interest to use methane as an alternative fuel to coal and oil due to its high ratio of hydrogen to carbon which leads to comparatively lower greenhouse gas emissions. First principle calculations suggest the fractures, which occur at weak joints within the 3DOM architecture, afford a large area of (001) surface that displays a reduced energy barrier for hydrogen abstraction, thereby facilitating methane oxidation. The hexapod-shaped perovskite catalyst exhibits excellent low temperature methane oxidation activity ( T 90%=438 ☌ reaction rate=4.84 × 10 −7 mol m −2 s −1).
On fragmenting three-dimensionally ordered macroporous (3DOM) structures in a controlled manner, via a process that has been likened to retrosynthesis, hexapod-shaped building blocks can be harvested which possess a mesostructured architecture. Here we show how the disassembly of an ordered porous La 0.6Sr 0.4MnO 3 perovskite array, to give hexapod mesostructured nanoparticles, exposes a new crystal facet which is more active for catalytic methane combustion. However, little information is known on how the structural disassembly influences the catalytic performance of the materials. App Package: superstructures composed of nanoparticles have recently been prepared using various disassembly methods.
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