Improving Syngas Selectivity of Fe2O3/Al2O3 with Yttrium Modification in Chemical Looping Methane Conversion
Kang, Yu1,2; Tian, Ming1; Huang, Chuande1; Lin, Jian1; Hou, Baolin1; Pan, Xiaoli1; Li, Lin1; Rykov, Alexandre I.1; Wang, Junhu1; Wang, Xiaodong1
刊名ACS CATALYSIS
2019-09-01
卷号9期号:9页码:8373-8382
关键词CH4 conversion chemical looping reforming Fe-based OCs garnet oxygen vacancy formation energy
ISSN号2155-5435
DOI10.1021/acscatal.9b02730
通讯作者Tian, Ming(tm1982@dicp.ac.cn) ; Wang, Xiaodong(xdwang@dicp.ac.cn)
英文摘要It is of great significance to improve the syngas selectivity of Fe-based oxygen carriers (OCs), because of their sufficient lattice oxygen, low cost, and environmental compatibility in chemical looping partial oxidation of CH4. In this work, it was found that the addition of Y could remarkably increase CO selectivity of Fe2O3/Al2O3 to 98% with a CH4 conversion of , similar to 90%. X-ray diffraction (XRD) and transmission electron microscopy (TEM) characterizations combined with Mossbauer spectroscopy illustrated that the incorporation of Y led to the Fe species gradually transferring from Fe2O3 into the garnet structure (Y3Fe2Al3O12), a newly formed phase, which was found to be highly active for syngas generation. Density functional theory (DFT) calculations demonstrated that such a high CO selectivity of confined Fe species in garnet originated from enhanced oxygen vacancy formation energy (E-ov), compared with Fe2O3, which resulted from the lattice oxygen shared by not only reducible Fe ions but also nonreducible Al and Y ones in a garnet structure. Therefore, our work provides a meaningful guidance of new materials screening for methane partial oxidation in the chemical looping process.
资助项目National Science Foundation of China (NSFC)[21406225] ; National Science Foundation of China (NSFC)[21573232] ; National Science Foundation of China (NSFC)[21676269] ; National Science Foundation of China (NSFC)[21706254] ; Postdoctoral Science Foundation of China[2014M561261]
WOS关键词PEROVSKITE-TYPE OXIDES ; PARTIAL OXIDATION ; OXYGEN CARRIERS ; SYNTHESIS GAS ; REDOX CATALYSTS ; HIGH-PERFORMANCE ; LATTICE OXYGEN ; CO2 CONVERSION ; MIXED OXIDES ; COMBUSTION
WOS研究方向Chemistry
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000485090400074
资助机构National Science Foundation of China (NSFC) ; National Science Foundation of China (NSFC) ; Postdoctoral Science Foundation of China ; Postdoctoral Science Foundation of China ; National Science Foundation of China (NSFC) ; National Science Foundation of China (NSFC) ; Postdoctoral Science Foundation of China ; Postdoctoral Science Foundation of China ; National Science Foundation of China (NSFC) ; National Science Foundation of China (NSFC) ; Postdoctoral Science Foundation of China ; Postdoctoral Science Foundation of China ; National Science Foundation of China (NSFC) ; National Science Foundation of China (NSFC) ; Postdoctoral Science Foundation of China ; Postdoctoral Science Foundation of China
内容类型期刊论文
源URL[http://cas-ir.dicp.ac.cn/handle/321008/172899]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Tian, Ming; Wang, Xiaodong
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, 19 A Yuquan Rd, Beijing 100049, Peoples R China
推荐引用方式
GB/T 7714
Kang, Yu,Tian, Ming,Huang, Chuande,et al. Improving Syngas Selectivity of Fe2O3/Al2O3 with Yttrium Modification in Chemical Looping Methane Conversion[J]. ACS CATALYSIS,2019,9(9):8373-8382.
APA Kang, Yu.,Tian, Ming.,Huang, Chuande.,Lin, Jian.,Hou, Baolin.,...&Wang, Xiaodong.(2019).Improving Syngas Selectivity of Fe2O3/Al2O3 with Yttrium Modification in Chemical Looping Methane Conversion.ACS CATALYSIS,9(9),8373-8382.
MLA Kang, Yu,et al."Improving Syngas Selectivity of Fe2O3/Al2O3 with Yttrium Modification in Chemical Looping Methane Conversion".ACS CATALYSIS 9.9(2019):8373-8382.
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