Impact of fuel-derived chlorine on CuO-based oxygen carriers for chemical looping with oxygen uncoupling

Journal Article · Mon Dec 09 00:00:00 EST 2019 · Fuel

DOI:https://doi.org/10.1016/j.fuel.2019.116780· OSTI ID:1799884

Dai, Jinze  ^[1]; Whitty, Kevin J. ^[1]

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1. Univ. of Utah, Salt Lake City, UT (United States)

During the chemical looping with oxygen uncoupling (CLOU) process for CO₂ capture from solid fuels, CuO-based oxygen carriers are expected to efficiently transport oxygen from the air reactor and convert fuel in the fuel reactor by releasing gaseous oxygen. To maintain high fuel conversion and CO₂ capture efficiency, it is important to understand the impact of the fuel-derived Cl, which is highly volatile and corrosive, on the CuO/Cu₂O in a CLOU environment. In this work, thermodynamic modeling was carried out to predict the characteristics of Cu-Cl interaction and develop a Cu deactivation rate model. Combustion experiments were performed to examine the impact of the Cl-containing flue gas on the CuO-based oxygen carrier. The oxygen transport capacities of the oxygen carriers exposed to the Cl-containing flue gas were measured by TGA. XRD and SEM-EDS were employed to characterize the ashes and oxygen carrier particles, respectively. The modeling results suggest that Cu-Cl interaction leads to the formation of CuCl and Cu₃Cl₃, causing the loss of effective Cu. The fraction of HCl converted to CuCl/Cu₃Cl₃ (X_HCl) was predicted to be almost linearly correlated with the Cl content, while H₂O could hinder the Cu-Cl interaction. The Cu deactivation rate model was successfully developed. For the fuels containing 0.2–0.4 wt% Cl, the Cu loss rate was estimated to be 0.0025–0.01%/cycle with X_HCl = 0.12–0.24. The results of combustion experiments and material characterization were consistent with the modeling predictions, clearly demonstrating the Cl-induced deactivation. Given the modeling predictions and experimental findings, potential countermeasures were proposed.

• Research Organization: Univ. of Utah, Salt Lake City, UT (United States)
• Sponsoring Organization: USDOE Office of Fossil Energy (FE)
• Grant/Contract Number: FE0029160
• OSTI ID: 1799884
• Alternate ID(s): OSTI ID: 1580637
• Journal Information: Fuel, Vol. 263; ISSN 0016-2361
• Publisher: Elsevier
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
chemical looping
CLOU
chlorine
CuO
thermodynamic modeling