Enhanced methane conversion in chemical looping partial oxidation systems using a copper doping modification

被引:123
作者
Qin, Lang [1 ]
Guo, Mengqing [1 ]
Liu, Yan [1 ]
Cheng, Zhuo [1 ]
Fan, Jonathan A. [2 ]
Fan, Liang-Shih [1 ]
机构
[1] Ohio State Univ, William G Lowrie Dept Chem & Biomol Engn, 151 W Woodruff Ave, Columbus, OH 43210 USA
[2] Stanford Univ, Spilker Engn & Appl Sci, Dept Elect Engn, Ginzton Lab, 348 Via Pueblo Mall, Stanford, CA 94305 USA
关键词
Chemical looping partial oxidation; Methane; Syngas; Iron-based carrier; Copper doping; TOTAL-ENERGY CALCULATIONS; OXIDE OXYGEN CARRIERS; SYNTHESIS GAS; LATTICE OXYGEN; SURFACE; METALS; XPS; CU;
D O I
10.1016/j.apcatb.2018.04.072
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Chemical looping partial oxidation (CLPO) is a promising strategy of methane conversion to syngas with low cost and minimal environmental impact. A major challenge is the development of oxygen carriers that have high reactivity, high oxygen carrying capacity, and recyclability. We demonstrate that the addition of a low concentration (1%) of copper dopant to iron-based oxygen carriers can dramatically enhance the reactivity in CLPO process at low temperatures while maintaining the recyclability of these carriers. With the dopant, the methane conversion rate at 700 degrees C is 470% higher than that of carriers without the dopant. These results are substantiated by ab initio DFT + U and thermochemistry analyses. It is noted that operating a chemical looping system at 700 degrees C can result in energy consumption savings of similar to 35% as compared to a chemical looping operation at 1000 degrees C. Thus, our findings provide a pathway to significantly lowering the methane reaction temperature in chemical looping systems, which will lead to substantial energy savings with desired oxygen carrier recyclability.
引用
收藏
页码:143 / 149
页数:7
相关论文
共 31 条
[1]   DENSITY-FUNCTIONAL CALCULATION OF EFFECTIVE COULOMB INTERACTIONS IN METALS [J].
ANISIMOV, VI ;
GUNNARSSON, O .
PHYSICAL REVIEW B, 1991, 43 (10) :7570-7574
[2]   Resolving surface chemical states in XPS analysis of first row transition metals, oxides and hydroxides: Sc, Ti, V, Cu and Zn [J].
Biesinger, Mark C. ;
Lau, Leo W. M. ;
Gerson, Andrea R. ;
Smart, Roger St. C. .
APPLIED SURFACE SCIENCE, 2010, 257 (03) :887-898
[3]   X-ray photoelectron spectroscopic chemical state quantification of mixed nickel metal, oxide and hydroxide systems [J].
Biesinger, Mark C. ;
Payne, Brad P. ;
Lau, Leo W. M. ;
Gerson, Andrea ;
Smart, Roger St. C. .
SURFACE AND INTERFACE ANALYSIS, 2009, 41 (04) :324-332
[4]   Oxygen vacancy promoted methane partial oxidation over iron oxide oxygen carriers in the chemical looping process [J].
Cheng, Zhuo ;
Qin, Lang ;
Guo, Mengqing ;
Xu, Mingyuan ;
Fan, Jonathan A. ;
Fan, Liang-Shih .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2016, 18 (47) :32418-32428
[5]  
Cheng Z, 2016, PHYS CHEM CHEM PHYS, V18, P16423, DOI [10.1039/c6cp01287f, 10.1039/c6cp012B7f]
[6]   Propagation of Olefin Metathesis to Propene on WO3 Catalysts: A Mechanistic and Kinetic Study [J].
Cheng, Zhuo ;
Lo, Cynthia S. .
ACS CATALYSIS, 2015, 5 (01) :59-72
[7]   Chemically and physically robust, commercially-viable iron-based composite oxygen carriers sustainable over 3000 redox cycles at high temperatures for chemical looping applications [J].
Chung, Cheng ;
Qin, Lang ;
Shah, Vedant ;
Fan, Liang-Shih .
ENERGY & ENVIRONMENTAL SCIENCE, 2017, 10 (11) :2318-2323
[8]  
Fan L.-S., 2017, Chemical Looping Partial Oxidation Gasification, Reforming, and Chemical Syntheses
[9]   Partial oxidation of methane to synthesis gas: Elimination of gas phase oxygen [J].
Fathi, M ;
Bjorgum, E ;
Viig, T ;
Rokstad, OA .
CATALYSIS TODAY, 2000, 63 (2-4) :489-497
[10]   Synthesis Gas Generation by Chemical-Looping Reforming Using Ce-Based Oxygen Carriers Modified with Fe, Cu, and Mn Oxides [J].
He, Fang ;
Wei, Yonggang ;
Li, Haibin ;
Wang, Hua .
ENERGY & FUELS, 2009, 23 (3-4) :2095-2102