Optimizing the sulfur-resistance and activity of perovskite oxygen carrier for chemical looping dry reforming of methane  

作　　者：Yuelun Li Dong Tian Lei jiang Huicong Zuo LiNan Huang Mingyi Chen Jianchun Zuo Hua Wang Kongzhai Li 

机构地区：[1]Engineering Research Center of Metallurgical Energy Conservation and Emission Reduction,Ministry of Education,Kunming University of Science and Technology,Kunming 650093,Yunnan,China [2]Faculty of Metallurgical and Energy Engineering,Kunming University of Science and Technology,Kunming 650093,Yunnan,China [3]State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization,Kunming University of Science and Technology,Kunming 650093,Yunnan,China

出　　处：《Journal of Energy Chemistry》2024年第9期259-271,共13页能源化学（英文版）

基　　金：financially supported by the National Natural Science Foundation of China (Nos. 52174279, U2202251, and 52266008);Applied Basic Research Program of Yunnan Province for Distinguished Young Scholars (No. 202201AV070004);Central Guiding Local Science and Technology Development Fund (No. 202207AA110001);the Yunnan Fundamental Research Projects (No. 202301AU070027, 202401AT070388)

摘　　要：Perovskite oxides has been attracted much attention as high-performance oxygen carriers for chemical looping reforming of methane,but they are easily inactivated by the presence of trace H_(2)S.Here,we propose to modulate both the activity and resistance to sulfur poisoning by dual substitution of Mo and Ni ions with the Fe-sites of LaFeO_(3)perovskite.It is found that partial substitution of Ni for Fe substantially improves the activity of LaFeO_(3)perovskite,while Ni particles prefer to grow and react with H_(2)S during the long-term successive redox process,resulting in the deactivation of oxygen carriers.With the presence of Mo in LaNi_(0.05)Fe_(0.95)O_(3−σ)perovskite,H_(2)S preferentially reacts with Mo to generate MoS_(2),and then the CO_(2)oxidation can regenerate Mo via removing sulfur.In addition,Mo can inhibit the accumulation and growth of Ni,which helps to improve the redox stability of oxygen carriers.The LaNi_(0.05)Mo_(0.07)Fe_(0.88)O_(3−σ)oxygen carrier exhibits stable and excellent performance,with the CH_(4)conversion higher than 90%during the 50 redox cycles in the presence of 50 ppm H_(2)S at 800℃.This work highlights a synergistic effect in the perovskite oxides induced by dual substitution of different cations for the development of high-performance oxygen carriers with excellent sulfur tolerance.

关 键 词：Perovskite oxygen carriers Chemical looping reforming Sulfur-resistance Dual substitution SYNGAS 

分 类 号：TE665.3[石油与天然气工程—油气加工工程] TB34[一般工业技术—材料科学与工程]