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Title: Unique phase identification of trimetallic copper iron manganese oxygen carrier using simultaneous differential scanning calorimetry/thermogravimetric analysis during chemical looping combustion reactions with methane

Chemical looping combustion (CLC) is a promising combustion technology that generates heat and sequestration-ready carbon dioxide that is undiluted by nitrogen from the combustion of carbonaceous fuels with an oxygen carrier, or metal oxide. This process is highly dependent on the reactivity and stability of the oxygen carrier. The development of oxygen carriers remains one of the major barriers for commercialization of CLC. Synthetic oxygen carriers, consisting of multiple metal components, have demonstrated enhanced performance and improved CLC operation compared to single metal oxides. However, identification of the complex mixed metal oxide phases that form after calcination or during CLC reactions has been challenging. Without an understanding of the dominant metal oxide phase, it is difficult to determine reaction parameters and the oxygen carrier reduction pathway, which are necessary for CLC reactor design. This is particularly challenging for complex multi-component oxygen carriers such as copper iron manganese oxide (CuFeMnO 4). This study aims to differentiate the unique phase formation of a highly reactive, complex trimetallic oxygen carrier, CuFeMnO 4, from its single and bimetallic counterparts using thermochemical and reaction data obtained from simultaneous differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) during temperature programmed reductions (TPR) with methane. DSC/TGA experimentsmore » during TPR with methane provides heat flow data and corresponding reaction rate data that can be used to determine reaction routes and mechanisms during methane reduction. Furthermore, non-isothermal TPR data provides the advantage of distinguishing reactions that may not be observable in isothermal analysis. The detailed thermochemical and reaction data, obtained during TPR with methane, distinguished a unique reduction pathway for CuFeMnO 4 that differed from its single and bimetallic counterparts. This is remarkable since X-ray diffraction (XRD) data alone could not be used to distinguish the reactive trimetallic oxide phase due to overlapping peaks from various single and mixed metal oxides. The unique reduction pathway of CuFeMnO 4 was further characterized in this study using in-situ XRD TPR with methane to determine changes in the dominant trimetallic phase that influenced the thermochemical and reaction rate data.« less
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [3]
  1. National Energy Technology Lab. (NETL), Morgantown, WV (United States); West Virginia Univ., Morgantown, WV (United States). Dept. of Chemical Engineering; Oak Ridge Inst. for Science and Education (ORISE), Oak Ridge, TN (United States)
  2. National Energy Technology Lab. (NETL), Morgantown, WV (United States)
  3. National Energy Technology Lab. (NETL), Morgantown, WV (United States); West Virginia Univ., Morgantown, WV (United States). Dept. of Chemical Engineering
Publication Date:
Report Number(s):
NETL-PUB-21098
Journal ID: ISSN 0306-2619; PII: S0306261917308140
Type:
Accepted Manuscript
Journal Name:
Applied Energy
Additional Journal Information:
Journal Volume: 203; Journal Issue: C; Journal ID: ISSN 0306-2619
Publisher:
Elsevier
Research Org:
National Energy Technology Lab. (NETL), Pittsburgh, PA, and Morgantown, WV (United States); Oak Ridge Inst. for Science and Education (ORISE), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Fossil Energy (FE)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Oxygen carriers; Chemical looping combustion; Phase identification
OSTI Identifier:
1440335