孟长功

个人信息Personal Information

教授

博士生导师

硕士生导师

性别:男

毕业院校:中科院金属所

学位:博士

所在单位:化工学院

学科:无机化学

办公地点:大连理工大学化学楼401

联系方式:13940825088

电子邮箱:cgmeng@dlut.edu.cn

扫描关注

论文成果

当前位置: 中文主页 >> 科学研究 >> 论文成果

Palladium Nanoparticles/Defective Graphene Composites as Oxygen Reduction Electrocatalysts: A First-Principles Study

点击次数:

论文类型:期刊论文

发表时间:2012-02-02

发表刊物:JOURNAL OF PHYSICAL CHEMISTRY C

收录刊物:SCIE、EI、Scopus

卷号:116

期号:4

页面范围:2710-2719

ISSN号:1932-7447

摘要:The impact of graphene substrate-Pd nanoparticle interaction on the O, OH, and OOH adsorption that is directly related to the electrocatalytic performance of these composites in oxygen reduction reaction (ORR) has been investigated by first-principles-based calculations. The calculated binding energy of a Pd-13 nanoparticle on a single vacancy graphene is as high as -6.10 eV, owing to the hybridization between the dsp states of the Pd particles with the sp(2) dangling bonds at the defect sites. The strong interaction results in the averaged d-band center of the deposited Pd nanoparticles shifted away from the Fermi level from -1.02 to -1.45 eV. Doping the single vacancy graphene with B or N will further tune the average d-band center and also the activity of the composite toward O, OH, and OOH adsorption. The adsorption energies of O, OH, and OOH are reduced from -4.78, -4.38, and -1.56 eV on the freestanding Pd-13 nanopartide to -4.57, -2.66, and -1.39 eV on Pd-13/single vacancy graphene composites, showing that the defective graphene substrate will not only stabilize the Pd nanoparticles but also reduce the adsorption energies of the O-containing species to the Pd particle, and so as the poisoning of the ORR active sites.