Interaction of O-2 with monolayer MoS2: Effect of doping and hydrogenation
Interaction of O-2 with monolayer MoS2: Effect of doping and hydrogenation
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O-2 与单层 MoS2 的相互作用：掺杂和氢化的影响
DOI：
10.1016/j.matdes.2016.10.005
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发表时间：
2017
影响因子：
8.4
通讯作者：
Tang Z.
中科院分区：
文献类型：
--
作者：
Zhao B.;Li T.;Qi N.;Chen Z. Q.;Liu L. L.;Cheng G. D.;Tang Z.
采用第一性原理计算结合CI-NEB方法研究了O2与掺杂单层MoS 2的相互作用以及氢化效应.通过掺杂Co、Ni和Cu原子可以打破MoS 2（001）面的表面化学惰性。在费米能级附近引入杂质能级，导致禁带宽度减小，有利于O2分子的吸附。活性氧原子是通过离解反应产生的。氢原子引入到掺杂MoS 2体系的表面，对O2的吸附和解离都产生了有利的影响。氢化后的MoS 2-Co/Ni体系中杂质能级增多，电子更多地集中在Co/Ni原子的3轨道上，表现出良好的吸附性能。加氢反应是通过氢吸附原子平稳地迁移到吸附的O2上形成OOH自由基而发生的。OOH自由基的O单键O键在较低的活化能势垒下解离，生成OH自由基和活性氧原子。理论研究表明，掺杂的单层MoS 2体系能有效地捕获O2分子，氢化作用促进了O2分子的吸附和解离.
The interaction of O2with doped monolayer MoS2and the effect of hydrogenation are studied by first-principles calculations coupled with the CI-NEB method. Surface chemically inertness of the MoS2(001) plane can be broken by doping with Co, Ni and Cu atoms. Impurity levels are induced around the Fermi level and lead to the decrease of band gap, which is beneficial to the adsorption of O2molecule. The activated oxygen atoms are produced through a dissociation reaction. The introduction of hydrogen atoms into the surface of doped MoS2system presents favorable effect for O2adsorption and dissociation. More impurity levels appear in the hydrogenated MoS2-Co/Ni system, and more electrons are localized at 3dorbital of Co/Ni atom, these systems all present excellent adsorption capacity. Hydrogenation reaction occurs by a hydrogen adatom smoothly migrating to the adsorbed O2with the formation of OOH radical. The elongated Osingle bondO bond of OOH radical can be dissociated with a lower activation energy barrier, producing an OH radical and activated oxygen atom. Our theoretical studies suggest that the doped monolayer MoS2system is effective for capturing O2molecule, and the hydrogenation is found to facilitate adsorption and dissociation of O2molecule.