α,β-不饱和醛在Ni-Pt(111)面上吸附的理论研究  

Theoretical Study on Adsorption of α,β-Unsaturated Aldehydes on Ni-Pt( 111) Surface

作　　者：罗伟 方镭 孟跃[2] 薛继龙[1] 陈涛 夏盛杰[1] 倪哲明[1] LUO Wei;FANG Lei;MENG Yue;XUE Jilong;CHEN Tao;XIA Shengjie;NI Zheming(College of Chemical Engineering,Zhejiang University of Technology,Hangzhou 310014,China;School of Life Sciences,Huzhou University,Huzhou 313000,China)

机构地区：[1]浙江工业大学化学工程学院,杭州310014 [2]湖州师范学院生命科学学院,湖州313000

出　　处：《高等学校化学学报》2019年第1期115-122,共8页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号:21503188);浙江省自然科学基金(批准号:LQ15B030002)资助~~

摘　　要：利用密度泛函理论研究了巴豆醛和肉桂醛分子在Pt-Ni-Pt(111)面的吸附构型以及相关电子性质.吸附构型与吸附能结果表明,巴豆醛和肉桂醛在覆盖度为1/25 ML的条件下,以C=C和C=O双键协同吸附在Pt-Ni-Pt(111)面较为稳定,且肉桂醛与Pt-Ni-Pt(111)面的吸附能远大于巴豆醛.由Mulliken电荷布局和差分电荷密度可知,在吸附过程中肉桂醛分子向Pt-Ni-Pt(111)面上转移的电荷数较巴豆醛更多,相互作用更大.由电子态密度分析结果可知,不饱和醛与Pt-Ni-Pt(111)面的吸附作用主要是由于分子的p轨道电子与催化剂d轨道电子之间的相互作用.由于苯基的存在使肉桂醛分子在Pt-Ni-Pt(111)面上的吸附更强,且平行于催化剂表面.The adsorption configurations of crotonaldehyde and cinnamaldehyde molecules on Pt-Ni-Pt(111)surface and their electronic properties were studied with density functional theory(DFT).The adsorption configurations and adsorption energy values illustrate that synergistic adsorption of crotonaldehyde and cinnamaldehyde molecules on Pt-Ni-Pt(111)surface with C O and C C bonds are most stable under the coverage of 1/25 ML.Moreover,the adsorption energy values of cinnamaldehyde on Pt-Ni-Pt(111)surface are much larger than that of crotonaldehyde.By analyzing Mulliken atomic charge population and the deformation density,it is found that the cinnamaldehyde molecule transfers more electrons to the Pt-Ni-Pt(111)surface and interact more strongly.The result of partial density of states(PDOS)indicates that the main reason for the adsorption is due to the interaction of the p orbital electrons of the unsaturated aldehyde molecules with the d orbital electrons of metal surface.And,due to the presence of the phenyl group,the cinnamaldehyde molecule is parallel to the surface of the Pt-Ni-Pt(111)and adsorbed more strongly.

关 键 词：密度泛函理论 巴豆醛 肉桂醛 Ni-Pt(111)面 吸附 

分 类 号：O641[理学—物理化学]