“…The morphological evolution of the calcined and CH 4 -CO 2 redox cycled samples is illustrated in Figure 2. The as-prepared 10Fe0Ni@Zr displays a hollow structure in a ZrO 2 matrix, as described elsewhere, 24 but this morphology disappears with addition of Ni. After 25 CH 4 -CO 2 redox cycles at 750 C, the microstructure of the 10FexNi@Zr samples is strongly modified, but 10Fe0Ni@Zr still maintains its hollow structure under the protection of ZrO 2 , which acts as a physical barrier to resist sintering.…”
Section: F I G U R Esupporting
confidence: 54%
“…In pure ZrO 2 , monoclinic and tetragonal zirconia are present in a 16:1 ratio. However, as indicated in previous work, 24 during the synthesis procedure of 10Fe0Ni@Zr, some Fe could get incorporated into the ZrO 2 phases, leading to more stabilization of the high‐temperature t‐polymorph. With the increment of Ni content, the Fe 2 O 3 phase peak gradually disappears, indicating redispersion into smaller particles takes place.…”
Section: Resultsmentioning
confidence: 68%
“…In order to calculate the oscillatory space–time yield (STY OSC , ), a dynamic simulation of chemical looping operation was performed based on the above 24 . This simulation is similar to a pressure‐swing process configured with multiple reactors, operating in parallel and switching between adsorption and regeneration.…”
Section: Methodsmentioning
confidence: 99%
“…In order to calculate the oscillatory space-time yield (STY OSC , mol H2=CO s À1 kg À1 FeþNi ), a dynamic simulation of chemical looping operation was performed based on the above STY H2=CO . 24 This simulation is similar to a pressure-swing process configured with multiple reactors, operating in parallel and switching between adsorption and regeneration. For the present work, 12 reactors were considered, each running in a chemical looping regime with feed valves switching between reductant and oxidant gas in a time delayed manner.…”
Section: In Situ Time Resolved Xrdmentioning
confidence: 99%
“…However, joining these two materials for chemical looping shows potential to achieve high activity and stability. 10,[20][21][22][23] In a previous study, 24 iron oxide with a special microstructure derived from Prussian blue was synthesized, namely nanostructured Fe 2 O 3 @ZrO 2 , which performed with high activity and stability in H 2 -CO 2 redox cycling. The objective of the present study is to apply this same material in CH 4 -CO 2 redox cycling.…”
CH 4 -CO 2 chemical looping is proposed for separate H 2 and CO production using nanostructured Fe-Ni looping materials. The product streams are obtained by first feeding CH 4 , which decomposes to H 2 and carbon. The latter acts as reductant for the subsequent CO 2 feed, which together with Fe re-oxidation yields CO. After 25 CH 4 -CO 2 cycles, 10Fe5Ni@Zr has a higher H 2 space-time yield than 10Fe0Ni@Zr (20 mmol s À1 kg À1FeþNi vs. 15 mmol s À1 kg À1 FeþNi ), a 2.6 times higher CO yield (57 mmol s À1 kg À1 FeþNi ) and lower deactivation. This improvement has two reasons: (i) CH 4 activation over Ni leading to cracking, (ii) product hydrogen causing deeper FeO reduction. Deactivation follows from accumulated carbon, non-reactive for CO 2 .On Ni and Fe sites, carbon can be removed by lattice oxygen or CO 2 , yielding more CO compared to the theoretical value for Fe oxidation. However, carbon that migrates away from the metals requires oxygen for removal, which restores the activity of the Ni-containing samples.carbon deposit, CH 4 -CO 2 redox cycling, chemical looping, CO 2 reduction, stability
| INTRODUCTIONCarbon dioxide (CO 2 ) and methane (CH 4 ) are two common greenhouse gases leading to climate change. [1][2][3] In view of environmental protection, the effective utilization of these two compounds is of global concern. [4][5][6] Fortunately, chemical looping provides a new framework to realize CO 2 reduction and CH 4 utilization with low exergy penalty and low economic cost. [7][8][9][10] In a chemical looping process, CO 2 and CH 4 can be converted into valuable chemicals through the cyclic reaction and regeneration of a looping mediator. For
“…The morphological evolution of the calcined and CH 4 -CO 2 redox cycled samples is illustrated in Figure 2. The as-prepared 10Fe0Ni@Zr displays a hollow structure in a ZrO 2 matrix, as described elsewhere, 24 but this morphology disappears with addition of Ni. After 25 CH 4 -CO 2 redox cycles at 750 C, the microstructure of the 10FexNi@Zr samples is strongly modified, but 10Fe0Ni@Zr still maintains its hollow structure under the protection of ZrO 2 , which acts as a physical barrier to resist sintering.…”
Section: F I G U R Esupporting
confidence: 54%
“…In pure ZrO 2 , monoclinic and tetragonal zirconia are present in a 16:1 ratio. However, as indicated in previous work, 24 during the synthesis procedure of 10Fe0Ni@Zr, some Fe could get incorporated into the ZrO 2 phases, leading to more stabilization of the high‐temperature t‐polymorph. With the increment of Ni content, the Fe 2 O 3 phase peak gradually disappears, indicating redispersion into smaller particles takes place.…”
Section: Resultsmentioning
confidence: 68%
“…In order to calculate the oscillatory space–time yield (STY OSC , ), a dynamic simulation of chemical looping operation was performed based on the above 24 . This simulation is similar to a pressure‐swing process configured with multiple reactors, operating in parallel and switching between adsorption and regeneration.…”
Section: Methodsmentioning
confidence: 99%
“…In order to calculate the oscillatory space-time yield (STY OSC , mol H2=CO s À1 kg À1 FeþNi ), a dynamic simulation of chemical looping operation was performed based on the above STY H2=CO . 24 This simulation is similar to a pressure-swing process configured with multiple reactors, operating in parallel and switching between adsorption and regeneration. For the present work, 12 reactors were considered, each running in a chemical looping regime with feed valves switching between reductant and oxidant gas in a time delayed manner.…”
Section: In Situ Time Resolved Xrdmentioning
confidence: 99%
“…However, joining these two materials for chemical looping shows potential to achieve high activity and stability. 10,[20][21][22][23] In a previous study, 24 iron oxide with a special microstructure derived from Prussian blue was synthesized, namely nanostructured Fe 2 O 3 @ZrO 2 , which performed with high activity and stability in H 2 -CO 2 redox cycling. The objective of the present study is to apply this same material in CH 4 -CO 2 redox cycling.…”
CH 4 -CO 2 chemical looping is proposed for separate H 2 and CO production using nanostructured Fe-Ni looping materials. The product streams are obtained by first feeding CH 4 , which decomposes to H 2 and carbon. The latter acts as reductant for the subsequent CO 2 feed, which together with Fe re-oxidation yields CO. After 25 CH 4 -CO 2 cycles, 10Fe5Ni@Zr has a higher H 2 space-time yield than 10Fe0Ni@Zr (20 mmol s À1 kg À1FeþNi vs. 15 mmol s À1 kg À1 FeþNi ), a 2.6 times higher CO yield (57 mmol s À1 kg À1 FeþNi ) and lower deactivation. This improvement has two reasons: (i) CH 4 activation over Ni leading to cracking, (ii) product hydrogen causing deeper FeO reduction. Deactivation follows from accumulated carbon, non-reactive for CO 2 .On Ni and Fe sites, carbon can be removed by lattice oxygen or CO 2 , yielding more CO compared to the theoretical value for Fe oxidation. However, carbon that migrates away from the metals requires oxygen for removal, which restores the activity of the Ni-containing samples.carbon deposit, CH 4 -CO 2 redox cycling, chemical looping, CO 2 reduction, stability
| INTRODUCTIONCarbon dioxide (CO 2 ) and methane (CH 4 ) are two common greenhouse gases leading to climate change. [1][2][3] In view of environmental protection, the effective utilization of these two compounds is of global concern. [4][5][6] Fortunately, chemical looping provides a new framework to realize CO 2 reduction and CH 4 utilization with low exergy penalty and low economic cost. [7][8][9][10] In a chemical looping process, CO 2 and CH 4 can be converted into valuable chemicals through the cyclic reaction and regeneration of a looping mediator. For
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