Rational Design of High-Performance DeNOx Catalysts Based on MnxCo3–xO4 Nanocages Derived from Metal–Organic Frameworks

Rational Design of High-Performance DeNOx Catalysts Based on MnxCo3–xO4 Nanocages Derived from Metal–Organic Frameworks
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DOI:
10.1021/cs401185c
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发表时间:
2014-05
期刊:
影响因子:
12.9
通讯作者:
Lei Zhang;Liyi Shi;Lei Huang;Jian-ping Zhang;R. Gao;Dengsong Zhang
Lei Zhang;Liyi Shi;Lei Huang;Jian-ping Zhang;R. Gao;Dengsong Zhang
中科院分区:
化学1区
文献类型:
--
作者:
Lei Zhang;Liyi Shi;Lei Huang;Jian-ping Zhang;R. Gao;Dengsong Zhang

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在此,我们合理地设计并首次开发了一种基于中空多孔MnxCo 3-xO 4纳米笼的高性能脱硝催化剂,该纳米笼具有由纳米立方体状金属有机骨架(Mn 3 [Co(CN)6]2·nH 2 O)热衍生的尖晶石结构,其通过自组装方法合成。所制备的催化剂进行了系统的表征,以阐明其形态结构和表面性质。与传统的MnxCo 3-xO 4纳米粒子相比,MnxCo 3-xO 4纳米笼具有更好的低温催化活性、更高的N2选择性、更宽的操作温度窗口、更高的稳定性和SO2耐受性。中空多孔结构的特点提供了更大的表面积和更多的活性位点来吸附和活化反应气体,从而导致高的催化活性。此外,锰和钴氧化物物种的均匀分布和强烈的相互作用不仅增强了催化循环,而且抑制了催化剂的形成。
Herein, we have rationally designed and originally developed a high-performance deNOx catalyst based on hollow porous MnxCo3–xO4 nanocages with a spinel structure thermally derived from nanocube-like metal–organic frameworks (Mn3[Co(CN)6]2·nH2O), which are synthesized via a self-assemble method. The as-prepared catalysts have been characterized systematically to elucidate their morphological structure and surface properties. As compared with conventional MnxCo3–xO4 nanoparticles, MnxCo3–xO4 nanocages possess a much better catalytic activity at low-temperature regions, higher N2 selectivity, more extensive operating-temperature window, higher stability, and SO2 tolerance. The feature of hollow and porous structures provides a larger surface area and more active sites to adsorb and activate reaction gases, resulting in the high catalytic activity. Moreover, the uniform distribution and strong interaction of manganese and cobalt oxide species not only enhance the catalytic cycle but also inhibit the formatio...