CO_(2) hydrogenation using protonic ceramic electrolysis cells(PCECs)to produce fuel gases such as CH_(4)and CO has been considered as a promising technology for effective CO_(2) utilization.However,the long-term stab...CO_(2) hydrogenation using protonic ceramic electrolysis cells(PCECs)to produce fuel gases such as CH_(4)and CO has been considered as a promising technology for effective CO_(2) utilization.However,the long-term stability of conventional PCECs based on Y and Yb doped BaZrO_(3)-BaCeO_(3)(BCZYYb)proton conductors is severely limited by their susceptibility to carbonate formation under high concentration CO_(2) .In this work,a new type PCEC based on CO_(2) -tolerant La_(5.6)WO_(11.4-δ)(LWO)material is firstly constructed.A three-layer porous-dense-porous LWO ceramic scaffold is fabricated via a pressing,dip-coating and cosintering process,followed by Ni and La_(0.6)Sr_(0.4)CoO_(3-δ)(LSC)catalyst impregnation to ensure the chemical compatibility among materials and form an efficient PCEC-based CO_(2) hydrogenation reactor.Benefits from the synergistic catalysis of nano nickel and LWO,the reactor gets a CH_(4)selectivity of over 50%at 600℃under 20%CO_(2) concentration,and it operates stably for over 320 h at 600–650℃under high CO_(2) concentrations of 50–80%,showing no degradation in CO_(2) conversion rate or CH_(4)selectivity.Postmortem analysis demonstrates that the CO_(2) absorption characteristics of LWO and the morphological uniformity of nano nickel lead to stable CO_(2) methanation.This study provides a viable strategy for designing highly stable PCEC-based CO_(2) hydrogenation reactors.展开更多
基金financially supported by the National Key R&D Program of China(2024YFF0506302)the National Natural Science Foundation of China(52372246)+1 种基金the Frontier Technologies R&D Program of Jiangsu(BF2024041)the Shanghai Engineering Research Center of Inorganic Energy Materials and Electric Power Sources(18DZ2280800)。
文摘CO_(2) hydrogenation using protonic ceramic electrolysis cells(PCECs)to produce fuel gases such as CH_(4)and CO has been considered as a promising technology for effective CO_(2) utilization.However,the long-term stability of conventional PCECs based on Y and Yb doped BaZrO_(3)-BaCeO_(3)(BCZYYb)proton conductors is severely limited by their susceptibility to carbonate formation under high concentration CO_(2) .In this work,a new type PCEC based on CO_(2) -tolerant La_(5.6)WO_(11.4-δ)(LWO)material is firstly constructed.A three-layer porous-dense-porous LWO ceramic scaffold is fabricated via a pressing,dip-coating and cosintering process,followed by Ni and La_(0.6)Sr_(0.4)CoO_(3-δ)(LSC)catalyst impregnation to ensure the chemical compatibility among materials and form an efficient PCEC-based CO_(2) hydrogenation reactor.Benefits from the synergistic catalysis of nano nickel and LWO,the reactor gets a CH_(4)selectivity of over 50%at 600℃under 20%CO_(2) concentration,and it operates stably for over 320 h at 600–650℃under high CO_(2) concentrations of 50–80%,showing no degradation in CO_(2) conversion rate or CH_(4)selectivity.Postmortem analysis demonstrates that the CO_(2) absorption characteristics of LWO and the morphological uniformity of nano nickel lead to stable CO_(2) methanation.This study provides a viable strategy for designing highly stable PCEC-based CO_(2) hydrogenation reactors.