Effect of Regeneration Period on the Selectivity of Synthesis Gas of Ba-Hexaaluminates in Chemical Looping Partial Oxidation of Methane

doi:10.1021/acscatal.8b03855

	Effect of Regeneration Period on the Selectivity of Synthesis Gas of Ba-Hexaaluminates in Chemical Looping Partial Oxidation of Methane
	Wang, Junhu 2; Shen, Qianqian 2,3; Huang, Fei 1; Tian, Ming 2; Zhu, Yanyan 3; Li, Lin 2; Wang, Xiaodong 2
刊名	ACS CATALYSIS
	2019
卷号	9 期号:1 页码:722-731
关键词	CH4 conversion chemical looping partial oxidation improvement of syngas regeneration period Ba-hexaaluminate
ISSN号	2155-5435
DOI	10.1021/acscatal.8b03855
通讯作者	Tian, Ming(tm1982@dicp.ac.cn) ; Zhu, Yanyan(yanyanzhu2006@126.com) ; Wang, Xiaodong(xdwang@dicp.ac.cn)
英文摘要	Chemical looping partial oxidation of CH4 is a promising method for producing syngas with a suitable H-2/CO ratio and avoiding the risk of explosion and use of an expensive air separation plant. However, regeneration of reduced oxygen carriers (OCs) by O-2 usually leads to the enrichment of surface electrophilic O2- or O- species and thus CO2 formation and a decrease in total CO selectivity. In this work, it was found that the CO selectivity of the BaFe3Al9O19 hexaaluminate (BF(3)A) OC was greatly improved from 58% to 83% by tuning the regeneration period, with a CH4 conversion of 86%, an H-2/CO ratio of 2, and a syngas yield of 4.2 mmol/g without significant carbon deposition. This resulted from the decrease in regeneration time (from 15 to 4.2 min), leading to a decrease in Fe3+ in Al(1), Al(2), and Al(3) sites (Fe-1, Fe-2, and Fe-3) active for combustion of CH4 and an increase in reduced Fe2+ to Fe-0 responsible for the partial oxidation of CH4. Consequently, the amount of CO2 decreased while that of CO increased significantly. In addition, unoxidized surface Fe-0 resulting from shorter regeneration periods (5 and 4.2 min) acted as catalysts for dry reforming of CH4 and CO2 at the beginning of the reaction, which also contributed to the increase in CO formation for these two samples.
资助项目	National Science Foundation of China (NSFC)[21303137] ; 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] ; National Science Foundation of China (NSFC)[21808033] ; Postdoctoral Science Foundation of China[2014M561261]
WOS关键词	SHELL REDOX CATALYST ; BARIUM HEXAALUMINATE ; OXYGEN-CARRIER ; CRYSTALLOGRAPHIC SITES ; MIXED OXIDES ; FE ; SYNGAS ; PERFORMANCE ; PEROVSKITES ; CONVERSION
WOS研究方向	Chemistry
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000455286600074
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/321008/166192]
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; Zhu, Yanyan; Wang, Xiaodong
作者单位	1.Fujian Normal Univ, 8 Shangsan Rd, Fuzhou 350007, Fujian, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, 457 Zhongshan Rd, Dalian 116023, Peoples R China 3.Northwest Univ, Coll Chem Engn, 229 Taibai Bei Rd, Xian 710069, Shaanxi, Peoples R China
推荐引用方式 GB/T 7714	Wang, Junhu,Shen, Qianqian,Huang, Fei,et al. Effect of Regeneration Period on the Selectivity of Synthesis Gas of Ba-Hexaaluminates in Chemical Looping Partial Oxidation of Methane[J]. ACS CATALYSIS,2019,9(1):722-731.
APA	Wang, Junhu.,Shen, Qianqian.,Huang, Fei.,Tian, Ming.,Zhu, Yanyan.,...&Wang, Xiaodong.(2019).Effect of Regeneration Period on the Selectivity of Synthesis Gas of Ba-Hexaaluminates in Chemical Looping Partial Oxidation of Methane.ACS CATALYSIS,9(1),722-731.
MLA	Wang, Junhu,et al."Effect of Regeneration Period on the Selectivity of Synthesis Gas of Ba-Hexaaluminates in Chemical Looping Partial Oxidation of Methane".ACS CATALYSIS 9.1(2019):722-731.