Remarkably Strong Chemisorption of Nitric Oxide on Insulating Oxide Films Promoted by Hybrid Structure,The Journal of Physical Chemistry C

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Remarkably Strong Chemisorption of Nitric Oxide on Insulating Oxide Films Promoted by Hybrid Structure
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2017-09-20 00:00:00 , DOI: 10.1021/acs.jpcc.7b06912
Zhenjun Song ₁ , Bin Zhao ₁ , Hu Xu ₂ , Peng Cheng ₁

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We report herein the remarkably strong chemical adsorption behaviors of nitric oxide on magnesia (001) film deposited on metal substrate by employing periodic density functional calculations with van der Waals corrections. As far as we know, the strong chemical adsorption of a single molecular nitric oxide over perfect inert oxide insulators such as magnesia has not yet been reported, without introduction of defects or morphological irregularities. Unlike the very weak physical interaction between nitric oxide and perfect magnesia, the molybdenum-supported magnesia (001) enhances adsorption capacities significantly, and the nitric oxide is chemisorbed strongly and preferably trapped in a flat adsorption configuration on metal-supported oxide film, due to the substantially large adsorption energies (1.65 eV) and transformation barrier heights. Bader charge populations, projected density of states, differential charge densities, electron localization function, and typical occupied orbitals are analyzed to uncover the electronic properties and nature of bonding between nitric oxide and surface as well as the bonding within the magnesia–molybdenum hybrid structure. Nitric oxide in flat configurations gains more electrons than that in bridge and top configurations, which is responsible for the largest adsorption strength in flat configuration. On the whole, the thinner oxide films are more severely oxidized, leading to the remarkably enhanced activity of monolayer magnesia (001). The strong chemical binding interaction between nitric oxide and magnesia deposited on a molybdenum slab offers new opportunities for toxic gas detection and treatment. We anticipate that the hybrid-structure-promoted remarkable chemical adsorption of nitric oxide on magnesia in this study will provide an inspiring clue for enhancing chemical activity and properties of insulating oxide.

中文翻译：

一氧化氮在混合结构促进的绝缘氧化膜上的强烈化学吸附

我们在此报告通过采用范德华校正的周期性密度泛函计算，一氧化氮在沉积在金属基底上的氧化镁（001）膜上的化学吸附行为非常强。据我们所知，尚未报道过在完美的惰性氧化物绝缘体（例如氧化镁）上单分子一氧化氮的强化学吸附，而没有引入缺陷或形态上的不规则性。与一氧化氮和完全氧化镁之间非常弱的物理相互作用不同，钼负载的氧化镁（001）显着提高了吸附能力，由于以下原因，一氧化氮被强烈地化学吸附，并优选以平坦的吸附构型捕集在金属负载的氧化膜上很大的吸附能（1.65 eV）和转化势垒高度。分析了较差的电荷种群，预计的状态密度，差分电荷密度，电子定位功能和典型的占据轨道，以揭示一氧化氮与表面之间键合以及氧化镁与钼杂化结构内键合的电子性质和性质。平面构型中的一氧化氮比桥和顶部构型中的电子获得更多的电子，这是平板构型中最大的吸附强度的原因。总体而言，较薄的氧化膜会被更严重地氧化，从而导致单层氧化镁（001）的活性显着增强。一氧化氮与沉积在钼板上的氧化镁之间的强化学结合相互作用为有毒气体的检测和处理提供了新的机会。

更新日期：2017-09-20

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