外电场对NO在Graphene负载的Pd单原子上的吸附特性的调控.pdfVIP

外电场对NO在Graphene负载的 Pd单原子上的吸附特性的调控 摘 要 ：本研究中 ，通过基于密度泛函理论的第一性原理并考虑范德华力修正计算了 Graphene负载的Pd 单原子界面特性以及NO的吸附特性(包括吸附构型的结构参数、吸附能和电子结构等) ，并着重研究了电 场对其吸附特性的调控规律及其内在机理.结果表 ：1) NO在Pd/Graphene上能够形成较强的化学吸 附 ，吸附能为1.09 eV.吸附的NO分子中的N-0键拉长.Pd - d态与NO-p态的强杂化作用都表 NO 分子在Pd - Graphene上被活化.2)在电场作用下Graphene负载的单原子Pd上的电荷随施加的电场逐渐 变化.3)跟没有施加电场的NO吸附的体系相比 ，当对NO吸附体系施加沿Z正方向的电场时 ，NO的吸 附增加 ，吸附的NO从衬底获得更多的负电荷 ，而Pd所带的正电荷逐步减少 ；当对NO吸附体系施加沿Z 负方向的电场时 ，NO的吸附减弱 ，吸附的NO从衬底获得的负电荷逐渐减少 ，而Pd所带的正电荷逐步增 加.4)外加电场能够有效地调控NO的吸附特性 ，并调控NO与衬底之间的电荷转移进而调控其电子结构. 关键词 ：外电场 ；NO吸附 ；DFT-D；单原子 ；Pd - Graphene Tuning the adsorption properties of NO on P single atom supporte by Graphene Abstract: In this paper, using the DFT 一 D method to simulate the inlerfacial properties of the Pd/Graphene, the adsorption properties of NO on Pd/Graphene as well as the effect of the external electric field are studied. It is found that： 1) the adsorption of the NO on Pd/Graphene is very strong with big adsorption energy of 1. 09 eV, and the N-0 bond is enlarged during the adsorption. The strong hybridized interaction between Pd - d states and NO - p states is the origin of the strong interaction between NO and Pd/Grpahene. 2) The charge of the an­ chored Pd on Graphene is changed with the external electric field. 3 ) Compare with the systems without external electric field, the adsorption of the NO on Pd/Graphene would be enhanced during the external electric field a- long the Z direction, and the adsorbed NO gets more electrons from the support. Otherwise, the adsorption of the NO on Pd/Graphene would be shrunk during the external electric field along the adverse Z direction, and the ad­ sorbed NO gets less electrons from the support. 4) The external electric field could effectively tune the adsorption properties of