First principles prediction of CH4 reactivities with Co3O4 nanocatalysts of different morphologies

doi:10.1039/c7cp04516f

	First principles prediction of CH4 reactivities with Co3O4 nanocatalysts of different morphologies
	Wang, Shibin1,2,3 ; Zhao, Chengcheng1,2,3 ; Li, Shenggang1,3 ; Sun, Yuhan1,3
	2017-12-07
发表期刊	PHYSICAL CHEMISTRY CHEMICAL PHYSICS (IF:2.9[JCR-2023],3.0[5-Year])
ISSN	1463-9076
卷号	19 期号:45 页码:30874-30882
发表状态	已发表
DOI	10.1039/c7cp04516f
摘要	Co3O4 nanocatalysts have been experimentally shown to have excellent performance in catalyzing CH4 combustion. These nanocatalysts of different morphologies, such as nanoparticle/nanocube, nanorod/nanobelt, and nanoplate/nanosheet, were previously synthesized and characterized to mainly expose the (001), (011), and (112) surfaces, respectively, with distinct reactivities. In this study, rigorous first principles calculations were performed to investigate CH4 reactivities of the above Co3O4 surfaces of different terminations. CH4 dissociation was predicted to occur at the Co-O pair site on these surfaces. For each surface, the most reactive Co-O pair site was identified based on calculated energy barriers of the different active sites, which should contribute most significantly to the reactivity of that surface. The lowest energy barriers for the (001), (011), and (112) surfaces were predicted to be 0.96, 0.90, and 0.79 eV, respectively, suggesting CH4 reactivity to increase in that order for the different Co3O4 surfaces, consistent with the trend found experimentally for Co3O4 nanocatalysts of different morphologies. Direct comparison between the estimated and experimental CH4 reaction rates per gram of the nanocatalysts at 325 degrees C further indicate that their relative ratios were well reproduced by considering three main factors: the effective energy barrier for CH4 dissociation, the surface area of the nanocatalyst, and the number of independent active sites per unit surface area. The important influence of surface area on CH4 reactivity is also demonstrated by the significant difference in the reactivities of the nanocatalysts when exposing the same facet but with distinct surface areas.
收录类别	SCI
语种	英语
资助项目	Ministry of Science and Technology of China[2016YFA0202802]
WOS研究方向	Chemistry ; Physics
WOS类目	Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS记录号	WOS:000416054400060
出版者	ROYAL SOC CHEMISTRY
WOS关键词	CHEMICAL-VAPOR-DEPOSITION ; TOTAL-ENERGY CALCULATIONS ; AUGMENTED-WAVE METHOD ; ELASTIC BAND METHOD ; H BOND ACTIVATION ; OXIDE THIN-FILMS ; DFT PLUS U ; METHANE COMBUSTION ; ELECTRONIC-STRUCTURE ; CATALYTIC COMBUSTION
原始文献类型	Article
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://kms.shanghaitech.edu.cn/handle/2MSLDSTB/10045
专题	物质科学与技术学院物质科学与技术学院_特聘教授组_孙予罕组物质科学与技术学院_特聘教授组_李圣刚组物质科学与技术学院_硕士生物质科学与技术学院_博士生
通讯作者	Li, Shenggang
作者单位	1.Chinese Acad Sci, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai Adv Res Inst, 100 Haike Rd, Shanghai 201210, Peoples R China 2.Univ Chinese Acad Sci, 19 Yuquan Rd, Beijing 100049, Peoples R China 3.ShanghaiTech Univ, Sch Phys Sci & Technol, 393 Middle Huaxia Rd, Shanghai 201210, Peoples R China
第一作者单位	物质科学与技术学院
通讯作者单位	物质科学与技术学院
推荐引用方式 GB/T 7714	Wang, Shibin,Zhao, Chengcheng,Li, Shenggang,et al. First principles prediction of CH4 reactivities with Co3O4 nanocatalysts of different morphologies[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2017,19(45):30874-30882.
APA	Wang, Shibin,Zhao, Chengcheng,Li, Shenggang,&Sun, Yuhan.(2017).First principles prediction of CH4 reactivities with Co3O4 nanocatalysts of different morphologies.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,19(45),30874-30882.
MLA	Wang, Shibin,et al."First principles prediction of CH4 reactivities with Co3O4 nanocatalysts of different morphologies".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 19.45(2017):30874-30882.