Various cerium-based metal–organic frameworks (Ce-MOFs and CeZr-MOFs) and their derivatives (CeZrO complex oxide catalysts) with different structures and properties by modulating the organic ligands (i.e., trimesic acid (BTC), 1,2,4,5-benzenetetracarboxylic acid (PMA), and terephthalic acid (BDC)) and transition metal elements via the solvothermal method. The performance of these catalysts was tested in the diesel soot oxidation reaction. In contrast, morphology engineering and the introduction of heteroatom zirconium to modify CeO can significantly improve the catalytic activity and stability of the catalyst. Among them, the best CeZrO-BDC shows remarkable catalytic performance for soot oxidation, converting 90% of soot particles into CO at about 410 °C. A series of characterization results demonstrate that the engineering of morphology provides a highly active polycrystalline surface for the adhesion of reactants, and the electron transfer system caused by Zr doping weakens the Ce-O bond. With the help of their combined action, the exposed polycrystal surfaces greatly enhance the oxygen vacancy content and the ability to generate reactive oxygen species. The DFT investigations shows that the presence of Zr can weaken the Ce-O link, result in favorable defect structures, and the reactive oxygen species of formation were promoted. This study provides an idea for the design of non-precious metal catalysts with high activity and stability.

中文翻译：

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MOFs衍生的多面体配位Ce10-xZrxOy催化剂的设计策略以增强烟灰燃烧

通过调节有机配体（即均苯三酸（BTC）、1,2,4）获得不同结构和性能的各种铈基金属有机骨架（Ce-MOFs和CeZr-MOFs）及其衍生物（CeZrO复合氧化物催化剂） ,5-苯四甲酸（PMA）和对苯二甲酸（BDC））和过渡金属元素通过溶剂热法。这些催化剂的性能在柴油烟灰氧化反应中进行了测试。相比之下，形貌工程和引入杂原子锆对CeO进行改性可以显着提高催化剂的催化活性和稳定性。其中，最好的CeZrO-BDC对烟灰氧化表现出显着的催化性能，在410℃左右将90%的烟灰颗粒转化为CO。一系列表征结果表明，形貌工程为反应物的粘附提供了高活性的多晶表面，并且Zr掺杂引起的电子转移系统削弱了Ce-O键。在它们的共同作用下，暴露的多晶表面大大提高了氧空位含量和产生活性氧的能力。 DFT研究表明Zr的存在可以削弱Ce-O键，产生有利的缺陷结构，并促进活性氧的形成。该研究为高活性、稳定性的非贵金属催化剂的设计提供了思路。