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It is still a challenge to develop metal-based monolithic deNOx catalysts with high activity, mass transfer ability and stability. Herein, we proposed a convenient and versatile pathway for the synthesis of novel monolithic deNOx catalysts originating from the in situ immobilization of metal organic framework (MOF) precursors on Fe mesh. Interestingly, the morphology and composition of the catalysts could be modulated by adjusting the synthesis parameters, such as the synthesis time, ligands and precursors, while the characterization results revealed an improvement in oxygen vacancies and Brønsted acid sites led by the strong interaction between the uniformly distributed active Mn–Fe components. As a result, the novel monolithic catalysts demonstrated improved catalytic performance compared with traditional catalysts obtained by hydroxide precursors. This work sheds lights on the advantages of using MOF-derived materials in situ decorated on metal mesh as monolithic catalysts and paves a way to design new monolithic deNOx catalysts with excellent low-temperature catalytic activity for future efforts. [ABSTRACT FROM AUTHOR]

In this work, we have rationally designed and originally developed a novel monolith de-NOx catalyst with nickel foam as the carrier and three dimensional hierarchical MnO2@NiCo2O4 core–shell nanowire arrays in situ grown on the surface via a two-step hydrothermal process with a post calcination treatment. The catalysts were systematically examined by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, elemental mapping, ion sputtering thinning, X-ray photoelectron spectroscopy, inductively coupled plasma atomic emission spectroscopy, H2 temperature-programmed reduction, NH3/NO + O2 temperature-programmed desorption measurements and catalytic performance tests. The results indicate that the nanowire is composed of hollow NiCo2O4 spinel as the core and MnO2 nanoparticles as the shell layer. By ingeniously making the hierarchical Ni–Co oxide nanowires as the support for manganese oxides, the MnO2@NiCo2O4@Ni foam catalyst not only takes advantage of the high surface area of Ni–Co nanowires to achieve high loading amounts as well as high dispersion of manganese oxides, but also makes use of the synergistic catalytic effect between Ni, Co and Mn multiple oxides, and exhibits excellent low-temperature catalytic performance in the end. In addition, with the structure and morphology well maintained under long term steady isothermal operation, the catalyst is able to sustain high NO conversion and exhibits superior catalytic cycle stability and good H2O resistance. Considering all these favorable properties, the MnO2@NiCo2O4@Ni foam catalyst could serve as a promising candidate for the monolith de-NOx catalyst at low temperatures and the rational design of in situ synthesis of 3D hierarchical monolith catalysts also puts forward a new way for the development of environmental-friendly and highly active monolith de-NOx catalysts. [ABSTRACT FROM AUTHOR]