by Sicong Tian, Feng Yan, Zuotai Zhang, and Jianguo Jiang

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Presentation transcript:

by Sicong Tian, Feng Yan, Zuotai Zhang, and Jianguo Jiang Calcium-looping reforming of methane realizes in situ CO2 utilization with improved energy efficiency by Sicong Tian, Feng Yan, Zuotai Zhang, and Jianguo Jiang Science Volume 5(4):eaav5077 April 12, 2019 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 1 Illustration of the proposed in situ CO2 utilization process. Illustration of the proposed in situ CO2 utilization process. (A) Process schematic of the catalytic CaL reforming of methane, and the (B) micrometer-scale morphology and (C and D) nanoparticle information of the CaO-Ni bifunctional sorbent-catalyst (freshly reduced CaO/Ni_9) driving the proposed process. Sicong Tian et al. Sci Adv 2019;5:eaav5077 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 2 Metal-support interaction in the material. Metal-support interaction in the material. (A) XPS spectra corresponding to Ni 2p3/2 and (B) H2-TPR profiles of the prepared CaO-Ni bifunctional sorbent-catalysts. a.u., arbitrary units. Sicong Tian et al. Sci Adv 2019;5:eaav5077 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 3 Reaction identification on the CaO-Ni interface. Reaction identification on the CaO-Ni interface. (A to C) Temperature-programmed reactions on the surface of freshly reduced CaO/Ni_9 to identify the coupling reactions involved in the CaL methane reforming process. (D) Gibbs free energy of related reactions as a function of temperature. Sicong Tian et al. Sci Adv 2019;5:eaav5077 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 4 Reaction studies of the CaL methane reforming process. Reaction studies of the CaL methane reforming process. (A) Syngas yield and H2-to-CO molar ratio and (B) conversion efficiency of CO2 and CH4 along with their consumption molar ratio as a function of the cycle number using CaO/Ni_9. (C) Specific yield of H2 and CO (average yield per gram of the loaded Ni) along with their molar ratio and (D) average conversion efficiency of CO2 and CH4 along with their average consumption molar ratio during the 10 cycles as a function of the Ni/(Ca + Ni) molar ratio in the sorbent-catalyst. Sicong Tian et al. Sci Adv 2019;5:eaav5077 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 5 Comparison of decarbonation kinetics between the CaL methane reforming and separate CaL processes. Comparison of decarbonation kinetics between the CaL methane reforming and separate CaL processes. In situ XRD characterization for isothermal decarbonation of (A) CaCO3 in a N2 atmosphere, (B) CaCO3 in a CH4 atmosphere, and (C) carbonated CaO/Ni_9 in a CH4 atmosphere at 1073 K. (D) Decarbonation rate as a function of time at 1073 K. Sicong Tian et al. Sci Adv 2019;5:eaav5077 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

Fig. 6 Energetics of the CaL methane reforming process. Energetics of the CaL methane reforming process. (A) Energy consumption for CO2 utilization (ECO2, kilojoules per mole of CO2 converted) and (B) fuel requirement for syngas production (XCH4, moles of CH4 consumed per mole of syngas produced) as a function of carbonation and calcination temperatures. The black curve indicates the value corresponding to the application of conventional MDR using the CO2 supplied by conventional CaL. The solid red circle indicates the value corresponding to the operating temperatures of the CaL methane reforming process investigated in this study. Sicong Tian et al. Sci Adv 2019;5:eaav5077 Copyright © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).