Fe-substituted Ba-hexaaluminate with enhanced oxygen mobility for CO_2 capture by chemical looping combustion of methane
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摘要
While Fe-based oxygen carriers(OC) are regarded to be promising for chemical looping combustion(CLC),the decrease of CO_2 selectivity during deep reduction process and the severe agglomeration of Fe_2O_3 often occur after multiple redox cycles due to the low oxygen mobility.Herein,Fe-substituted Bahexaaluminates(Ba Fe_xAl_(12)– xO_(19),denoted as BF_xA-H,x = 1 and 2) prepared by a modified two-step method exhibited not only higher amount of converted oxygen(Ot) and CH_4 conversion(77% and 81% vs.17%and 75%) than those prepared by the traditional co-precipitation method(BF_xA-C,x = 1 and 2) but also high CO_2 selectivity above 92% during the nearly whole reduction from Fe~(3+) to Fe~(2+).Furthermore,the BFxA-H exhibited the excellent recyclability during 50 cycles.The better performance was ascribed to the markedly enhanced oxygen mobility which resulted from dominant occupancy of Fe cations in Al(5) sites(Fe~5: 71% and 70% vs.49% and 41%) in mirror planes of hexaaluminate leading to larger amount of lattice oxygen coordinated with Fe~5(O–Fe~5)(0.45 and 0.85 mmol/g vs.0.31 and 0.50 mmol/g).The improvement of oxygen mobility also favored the preservation of chemical state of Fe cations in hexaaluminate structure in the re-oxidation step,resulting in the excellent recyclability of BF_xA-H.
While Fe-based oxygen carriers(OC) are regarded to be promising for chemical looping combustion(CLC),the decrease of CO_2 selectivity during deep reduction process and the severe agglomeration of Fe_2O_3 often occur after multiple redox cycles due to the low oxygen mobility.Herein,Fe-substituted Bahexaaluminates(Ba Fe_xAl_(12)– xO_(19),denoted as BF_xA-H,x = 1 and 2) prepared by a modified two-step method exhibited not only higher amount of converted oxygen(Ot) and CH_4 conversion(77% and 81% vs.17%and 75%) than those prepared by the traditional co-precipitation method(BF_xA-C,x = 1 and 2) but also high CO_2 selectivity above 92% during the nearly whole reduction from Fe~(3+) to Fe~(2+).Furthermore,the BFxA-H exhibited the excellent recyclability during 50 cycles.The better performance was ascribed to the markedly enhanced oxygen mobility which resulted from dominant occupancy of Fe cations in Al(5) sites(Fe~5: 71% and 70% vs.49% and 41%) in mirror planes of hexaaluminate leading to larger amount of lattice oxygen coordinated with Fe~5(O–Fe~5)(0.45 and 0.85 mmol/g vs.0.31 and 0.50 mmol/g).The improvement of oxygen mobility also favored the preservation of chemical state of Fe cations in hexaaluminate structure in the re-oxidation step,resulting in the excellent recyclability of BF_xA-H.
While Fe-based oxygen carriers(OC) are regarded to be promising for chemical looping combustion(CLC),the decrease of CO_2 selectivity during deep reduction process and the severe agglomeration of Fe_2O_3 often occur after multiple redox cycles due to the low oxygen mobility.Herein,Fe-substituted Bahexaaluminates(Ba Fe_xAl_(12)– xO_(19),denoted as BF_xA-H,x = 1 and 2) prepared by a modified two-step method exhibited not only higher amount of converted oxygen(Ot) and CH_4 conversion(77% and 81% vs.17%and 75%) than those prepared by the traditional co-precipitation method(BF_xA-C,x = 1 and 2) but also high CO_2 selectivity above 92% during the nearly whole reduction from Fe~(3+) to Fe~(2+).Furthermore,the BFxA-H exhibited the excellent recyclability during 50 cycles.The better performance was ascribed to the markedly enhanced oxygen mobility which resulted from dominant occupancy of Fe cations in Al(5) sites(Fe~5: 71% and 70% vs.49% and 41%) in mirror planes of hexaaluminate leading to larger amount of lattice oxygen coordinated with Fe~5(O–Fe~5)(0.45 and 0.85 mmol/g vs.0.31 and 0.50 mmol/g).The improvement of oxygen mobility also favored the preservation of chemical state of Fe cations in hexaaluminate structure in the re-oxidation step,resulting in the excellent recyclability of BF_xA-H.
引文
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