Theoretical modeling of interactions of Cr2On and Mn2On clusters with H2 molecules

IF 2.5 4区 化学 Q4 BIOCHEMISTRY & MOLECULAR BIOLOGY
Konstantin V. Bozhenko, Andrey N. Utenyshev, Lavrenty G. Gutsev, Sergey M. Aldoshin, Gennady L. Gutsev
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Abstract

Context

Gas sensors with high sensitivity and selectivity are essential for industrial safety and environmental monitoring. The ongoing development of more effective sensors relies on two key aspects: the design of novel sensing materials and a deeper understanding of the underlying sensing mechanisms. Among the various materials used for the sensor fabrication, semiconducting metal oxides such as chromium and manganese oxides have garnered much recent attention. Notably, palladium-doped chromium oxide has demonstrated high efficiency in hydrogen sensing. Chromium oxides can function as single-component sensors and also in components of composite systems. Manganese oxides are likewise widely used in sensing applications, especially as electrochemical sensors either alone or in combination with other metal oxides.

Methods

All calculations were carried out by using spin-polarized density functional theory with the generalized gradient approximation as implemented in Gaussian 09. Among the numerous exchange–correlation functionals and basis sets, we chose the BPW91 functional and 6–311 + G* basis set of triple-zeta quality. We considered reactions of Cr2On and Mn2On with H2 and found pathways leading from the reagents to products. All but one reaction pathways were found to have two or three transition states separated by local minima. The search of transition states was performed by using the modified conjugate gradient algorithm and the local minima were determined by applying the intrinsic reaction coordinate algorithm. It was found that some of the pathways are spin-dependent, i.e., the total spin magnetic moments of reagents do not match those of the products.

Cr2On和Mn2On簇与H2分子相互作用的理论建模。
背景:具有高灵敏度和选择性的气体传感器对于工业安全和环境监测至关重要。更有效的传感器的持续发展依赖于两个关键方面:新型传感材料的设计和对潜在传感机制的深入了解。在用于传感器制造的各种材料中,半导体金属氧化物如铬和锰氧化物最近引起了人们的广泛关注。值得注意的是,钯掺杂氧化铬在氢传感方面表现出了很高的效率。氧化铬可以作为单组分传感器,也可以作为复合系统的组分。锰氧化物同样广泛用于传感应用,特别是作为电化学传感器单独或与其他金属氧化物组合。方法:所有计算均采用自旋极化密度泛函理论,并在Gaussian 09中实现广义梯度逼近。在众多的交换相关函数和基集中,我们选择了BPW91函数和6-311 + G*的triple-zeta质量基集。我们考虑了Cr2On和Mn2On与H2的反应,并找到了从试剂到产物的途径。除一种反应途径外,其余的反应途径都有两个或三个过渡态,由局部极小值隔开。采用改进的共轭梯度算法搜索过渡态,采用内禀反应坐标算法确定局部最小值。研究发现,有些反应途径是自旋依赖的,即试剂的总自旋磁矩与产物的总自旋磁矩不匹配。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Journal of Molecular Modeling
Journal of Molecular Modeling 化学-化学综合
CiteScore
3.50
自引率
4.50%
发文量
362
审稿时长
2.9 months
期刊介绍: The Journal of Molecular Modeling focuses on "hardcore" modeling, publishing high-quality research and reports. Founded in 1995 as a purely electronic journal, it has adapted its format to include a full-color print edition, and adjusted its aims and scope fit the fast-changing field of molecular modeling, with a particular focus on three-dimensional modeling. Today, the journal covers all aspects of molecular modeling including life science modeling; materials modeling; new methods; and computational chemistry. Topics include computer-aided molecular design; rational drug design, de novo ligand design, receptor modeling and docking; cheminformatics, data analysis, visualization and mining; computational medicinal chemistry; homology modeling; simulation of peptides, DNA and other biopolymers; quantitative structure-activity relationships (QSAR) and ADME-modeling; modeling of biological reaction mechanisms; and combined experimental and computational studies in which calculations play a major role.
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