Density functional studies of zirconia with different crystal phases for oxygen reduction reaction

被引：12

作者：

Wang, Guangjin ^{[1
,2
]}

Huang, Fei ^{[3
]}

Chen, Xiaobo ^{[4
]}

Wen, Sheng ^{[1
]}

Gong, Chunli ^{[1
]}

Liu, Hai ^{[1
]}

Cheng, Fan ^{[1
]}

Zheng, Xuan ^{[1
]}

Zheng, Genwen ^{[1
]}

Pan, Mu ^{[2
]}

机构：

[1] Hubei Engn Univ, Coll Chem & Mat Sci, Xiaogan 432000, Peoples R China

[2] Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Peoples R China

[3] Guangdong Acad Agr Sci, Sericultural & Agrifood Res Inst, Guangdong Key Lab Agr Prod Proc, Key Lab Funct Foods,Minist Agr, Guangzhou 510610, Guangdong, Peoples R China

[4] Jinan Univ, Coll Sci & Engn, Guangzhou 510632, Guangdong, Peoples R China

来源：

RSC ADVANCES | 2015年 / 5卷 / 103期

基金：

中国国家自然科学基金; 国家教育部博士点专项基金资助;

关键词：

MOLECULAR-DYNAMICS SIMULATION; AB-INITIO; SURFACES; ELECTROCATALYSTS; 1ST-PRINCIPLES; TRANSITION; ELECTROLYSIS; CARBON; WATER; O-2;

D O I：

10.1039/c5ra14731j

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

To understand the origin of its catalytic activity, the oxygen reduction reaction (ORR) on zirconia with different phases is investigated by the first principles method. The free energy diagrams for an associative mechanism are firstly given to identify the rate-determining step for the ORR on the (111) surface of monoclinic, tetragonal and cubic phase zirconia. The calculation results show that the first electron transfer is the rate-determining step for the ORR on monoclinic and cubic phase zirconia, whereas the last electron transfer is the rate-limiting step for the ORR on tetragonal phase zirconia. The d-electron partial density of states for the active zirconium atoms is calculated to explore the relationship between the ORR catalytic activity of zirconia with different phases and their electronic properties. The calculated results show that the catalytic activity of zirconia for ORR is strongly dependent on the d-orbital occupation of the active zirconium atoms.

引用

页码：85122 / 85127

页数：6

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