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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Reduction of NO to N2O Catalyzed by a Mn-Substituted Keggin-Type Polyoxometalate: A Density Functional Theory Study
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Reduction of NO to N2O Catalyzed by a Mn-Substituted Keggin-Type Polyoxometalate: A Density Functional Theory Study

机译：通过Mn取代的Keggin型聚氧酸盐催化的NO NO NO NO NO：密度函数理论研究

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摘要

Reaction mechanism corresponding to reduction of NO to N2O catalyzed by mono-transition-metal-substituted Keggin-type polyoxometalates (POMs) has been studied by using a density functional theory (DFT) method with the M06L functional. Compared with Fe-, Co-, and Zn-substituted POM complexes, a Mn-substituted POM complex possesses good feature for activation of NO molecule because of considerable absorption energy and significant charge transfer from metal center to NO molecule. The effective interaction between NO ligand and the Mn center mainly comes from an overlap of the pi* orbital of the NO molecule with d(xz) and d(z2) orbital of Mn center. Three possible reaction pathways for reduction of NO to N2O catalyzed by Mn-substituted POM complex have been considered based on a dimer mechanism. The calculated free energy profile indicates that the reaction pathway undergoing a cis-(NO)(2) conformation is the favorable route because of a low free energy barrier of 4.24 kcal mol(-1). This work would be very useful to guide the design of nitric oxide reduction catalyst based on inorganic POM complexes in fiend of environmental catalysis.
机译：通过使用M06L功能的密度泛函理论（DFT）方法研究了对应于单转化 - 金属取代的Keggin型多氧化嘧啶（POMS）催化的NO NO NO NO NO NO N 2 O的反应机制。与Fe-，Co-和Zn取代的POM络合物相比，Mn取代的POM络合物具有良好的特征，用于活化没有分子，因为从金属中心到没有分子的金属中心显着的电荷转移。无配体和Mn中心之间的有效相互作用主要来自PI *轨道的NO分子与Mn中心的D（XZ）和D（Z2）轨道的重叠。基于二聚体机制，已经考虑了用于减少由Mn取代的POM络合物催化的NO O至N 2 O的可能反应途径。计算的自由能曲线表明，由于4.24kcal摩尔（-1）的低自由能屏障，所经历CIS-（NO）（2）构象的反应途径是有利的路线。这项工作对于指导基于环境催化恶魔中的无机POM络合物的一氧化氮还原催化剂设计非常有用。

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