We have designed and elaborately fabricated the ordered hierarchical macro-meso-microporous catalysts of Ce_0.25Zr_0.75O₂-supported Pt-embedded KMnO_x nanoparticles (OMMM Pt-KMnO_x/Ce_0.25Zr_0.75O₂). Three dimensionally ordered macro-mesoporous (3DOMM) Ce_0.25Zr_0.75O₂ oxide was synthesized by the combined methods of evaporation-induced interfacial self-assembly (EISA) and colloidal crystal templates (CCT). KMnO_x nanoparticles (NPs) possess the natural microporous nanostructure of an octahedral molecular sieve (OMS) with an average size of 0.46 nm. Pt nanoclusters were anchored in situ at the microporous structure of KMnO_x NPs and formed Pt-KMnO_x active sites. For the OMMM Pt-KMnO_x/Ce_0.25Zr_0.75O₂ catalyst, a 3D ordered macroporous (250 nm) structure can enhance contact efficiency between soot and catalysts, and a high specific surface area with contributions from ordered mesopores (5 nm) is beneficial for dispersion of KMnO_x NPs and activation of gaseous reactants (O₂ and NO). Meanwhile, a microporous (0.46 nm) structure can anchor K sites and ultrafine Pt nanoclusters. The synergetic effect of ternary K-Mn-Pt components can transform gas reactants to the effective intermediate species and thereafter oxidize the well-dispersed soot particles. The OMMM Pt-KMnO_x/Ce_0.25Zr_0.75O₂ catalyst possesses high catalytic activity and stability for soot oxidation under the conditions of loose contact: i.e., its TOF value is 2.10 h^–1 at 290 °C, which is more than a 4-fold increase over the 3DOMM Ce_0.25Zr_0.75O₂ support (0.47 h^–1). The architected hierarchical porous structure rationalizes an alternative protocol to improve solid–solid contact and the resulting activity, which can be further applied to other catalysis systems with different catalysts and reactants.

中文翻译：

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有序分层多孔Pt-KMnO _x / Ce _0.25 Zr _0.75 O ₂催化剂中K位和Pt纳米簇的协同效应以促进烟So氧化

我们已经设计并精心制造了Ce _0.25 Zr _0.75 O ₂负载的Pt嵌入的KMnO _x纳米粒子（OMMM Pt-KMnO _x / Ce _0.25 Zr _0.75 O ₂）的有序的分层大介观微孔催化剂。采用蒸发诱导界面自组装（EISA）和胶体晶体模板（CCT）相结合的方法，合成了三维有序的大中观（3DOMM）Ce _0.25 Zr _0.75 O ₂氧化物。高锰酸钾_X纳米颗粒（NPs）具有八面体分子筛（OMS）的天然微孔纳米结构，平均尺寸为0.46 nm。Pt纳米团簇原位锚定在KMnO _x NPs的微孔结构上，并形成Pt-KMnO _x活性位点。对于OMMM Pt-KMnO _x / Ce _0.25 Zr _0.75 O ₂催化剂，3D有序大孔（250 nm）结构可以提高烟灰与催化剂之间的接触效率，并且高比表面积是由有序介孔（5 nm）贡献的。有利于KMnO _x NP的分散和气态反应物（O ₂和不）。同时，微孔（0.46 nm）结构可以锚定K位点和超细Pt纳米簇。三元K-Mn-Pt组分的协同作用可以将气体反应物转化为有效的中间物质，然后氧化分散良好的烟灰颗粒。OMMM Pt-KMnO _x / Ce _0.25 Zr _0.75 O ₂催化剂在松散接触条件下具有高催化活性和烟尘氧化稳定性：即，在290°C下的TOF值为2.10 h ^–1，大于比3DOMM Ce _0.25 Zr _0.75 O ₂支撑（0.47 h ^–1）。所设计的分层多孔结构合理化了替代方案，以改善固-固接触和所产生的活性，该方案可以进一步应用于具有不同催化剂和反应物的其他催化体系。