Reduction kinetics of SrFeO<sub>3−<i>δ</i></sub>/CaO∙MnO nanocomposite as effective oxygen carrier for chemical looping partial oxidation of methane

doi:10.1007/s11705-022-2188-5

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (12) : 1726-1734 https://doi.org/10.1007/s11705-022-2188-5

RESEARCH ARTICLE

Reduction kinetics of SrFeO_3−δ/CaO∙MnO nanocomposite as effective oxygen carrier for chemical looping partial oxidation of methane

Xinhe Wang¹, Liuqing Yang², Xiaolin Ji², Yunfei Gao^3,⁴, Fanxing Li⁴, Junshe Zhang²(

), Jinjia Wei^1,²(

)

¹. State Key Laboratory of Multiphase Flow in Power Engineering, Xi’an Jiaotong University, Xi’an 710049, China
². School of Chemical Engineering and Technology, Xi’an Jiaotong University, Xi’an 710049, China
³. Institute of Clean Coal Technology, East China University of Science and Technology, Shanghai 200237, China
⁴. Department of Chemical and Biomolecular Engineering, North Carolina State University, Raleigh, NC 27695, USA

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Abstract

Chemical looping reforming of methane is a novel and effective approach to convert methane to syngas, in which oxygen transfer is achieved by a redox material. Although lots of efforts have been made to develop high-performance redox materials, a few studies have focused on the redox kinetics. In this work, the kinetics of SrFeO_3−δ–CaO∙MnO nanocomposite reduction by methane was investigated both on a thermo-gravimetric analyzer and in a packed-bed microreactor. During the methane reduction, combustion occurs before the partial oxidation and there exists a transition between them. The weight loss due to combustion increases, but the transition region becomes less inconspicuous as the reduction temperature increased. The weight loss associated with the partial oxidation is much larger than that with combustion. The rate of weight loss related to the partial oxidation is well fitted by the Avrami–Erofeyev equation with n = 3 (A3 model) with an activation energy of 59.8 kJ∙mol^‒1. The rate law for the partial oxidation includes a solid conversion term whose expression is given by the A3 model and a methane pressure-dependent term represented by a power law. The partial oxidation is half order with respect to methane pressure. The proposed rate law could well predict the reduction kinetics; thus, it may be used to design and/or analyze a chemical looping reforming reactor.

Keywords chemical looping reforming SrFeO_3−δ/CaO·MnO nanocomposite reduction kinetics Avrami–Erofeyev model pressure-dependent term

Corresponding Author(s): Junshe Zhang,Jinjia Wei

Online First Date: 01 November 2022 Issue Date: 19 December 2022

Cite this article:

Xinhe Wang,Liuqing Yang,Xiaolin Ji, et al. Reduction kinetics of SrFeO_3−δ/CaO∙MnO nanocomposite as effective oxygen carrier for chemical looping partial oxidation of methane[J]. Front. Chem. Sci. Eng., 2022, 16(12): 1726-1734.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2188-5
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I12/1726

Fig.1 (a) TG, (b) DTG and (c) dX/dt vs. X curves of SF–CM reduction by methane at three temperatures, and (d) Arrhenius plot; reaction conditions: m_SF–CM = 27 mg, F = 110 STP?mL?min^?1 (10 vol % CH₄), P = 1 atm.

Fig.2 Schematic diagram of SF–CM reduction by methane.

Fig.3 Kinetics of SF–CM reduction at three methane partial pressures: (a) CO flowrate as a function of time, (b) conversion of redox material as a function of time, (c) plots of dX/dt vs. X, and (d) the plots of ln[?ln(1 ? X)] as function of time t; reaction conditions: m_SF–CM = 1 g, T = 900 °C, F = 110 STP?mL·min^?1, P = 1 atm.

Methane pressure/atm	ln( $k ′ P C H 4 β$ )	Expected runs	Number of runs
0.15	?6.2842	170	168
0.20	?61896	150	150
0.30	?5.9663	116	116
0.40	?5.7943	100	96
0.50	?5.7244	95	95

Tab.1 Values of ln(

k ′ P C H 4 β

) and runs test for 5 methane partial pressures

Fig.4 Plot of ln(

k ′ P C H 4 β

) vs. ln

P C H 4

Fig.5 The predicted and measured reduction rates for four methane partial pressures: (a) 0.15, (b) 0.30, (c) 0.40, and (d) 0.50 atm; reaction conditions: m_SF–CM = 1 g, T = 900 °C, F = 110 STP?mL?min^?1, P = 1 atm.

Fig.6 The Q–Q plot for four methane partial pressures: (a) 0.15, (b) 0.30, (c) 0.40, and (d) 0.50 atm; reaction conditions: m_SF–CM = 1 g, T = 900 °C, F = 110 STP?mL?min^?1, P = 1 atm.

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