锂氧电池高容量正极材料花球状碳微球的三维复刻构筑（英文）
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摘要
活性物质和电极的多孔结构设计是实现锂氧电池中氧气电极高容量和良好可逆性的关键措施.本文报道了一种创新的三维复刻策略,并用于设计锂氧电池氧气电极用多孔碳材料的三维结构.作为一个实例,采用聚多巴胺包覆层为碳源,通过完整复制纳米结构氧化锌模板的形貌,成功地制备了由扭曲的中空碳纳米片组装而成的花球状碳微球.作为氧气电极的活性物质,花球状碳微球的三维多孔结构不仅能容纳放电产物过氧化锂,同时也能保持离子和气体的扩散通道.此外,氮掺杂引入的高缺陷为氧还原/析出反应提供了充足的活性位点.从而,花球状碳微球表现出高达9163.7 mA h g~(-1)的比容量和优异的可逆性.本工作呈现了一种用于能源存储和转化的多孔碳材料的三维结构的有效可控制备方法,即复制过渡金属氧化物模板的纳米结构.
The robust porous architectures of active materials are highly desired for oxygen electrodes in lithium–oxygen batteries to enable high capacities and excellent reversibility. Herein, we report a novel three-dimensional replication strategy to fabricate three-dimensional architecture of porous carbon for oxygen electrodes in lithium–oxygen batteries. As a demonstration, ball-flower-like carbon microspheres assembled with tortuous hollow carbon nanosheets are successfully prepared by completely replicating the morphology of the nanostructured zinc oxide template and utilizing the polydopamine coating layer as the carbon source.When used as the active material for oxygen electrodes, the three-dimensional porous architecture of the prepared ballflower-like carbon microspheres can accommodate the discharge product lithium peroxide and simultaneously maintain the ions and gas diffusion paths. Moreover, their high degrees of defectiveness by nitrogen doping provide sufficient active sites for oxygen reduction/evolution reaction.Thus the prepared ball-flower-like carbon microspheres demonstrate a high capacity of 9,163.7 mA h g~(-1) and excellent reversibility. This work presents an effective way to prepare three-dimensional architectures of porous carbon by replicating the controllable nanostructures of transition metal oxide templates for energy storage and conversion applications.
The robust porous architectures of active materials are highly desired for oxygen electrodes in lithium–oxygen batteries to enable high capacities and excellent reversibility. Herein, we report a novel three-dimensional replication strategy to fabricate three-dimensional architecture of porous carbon for oxygen electrodes in lithium–oxygen batteries. As a demonstration, ball-flower-like carbon microspheres assembled with tortuous hollow carbon nanosheets are successfully prepared by completely replicating the morphology of the nanostructured zinc oxide template and utilizing the polydopamine coating layer as the carbon source.When used as the active material for oxygen electrodes, the three-dimensional porous architecture of the prepared ballflower-like carbon microspheres can accommodate the discharge product lithium peroxide and simultaneously maintain the ions and gas diffusion paths. Moreover, their high degrees of defectiveness by nitrogen doping provide sufficient active sites for oxygen reduction/evolution reaction.Thus the prepared ball-flower-like carbon microspheres demonstrate a high capacity of 9,163.7 mA h g~(-1) and excellent reversibility. This work presents an effective way to prepare three-dimensional architectures of porous carbon by replicating the controllable nanostructures of transition metal oxide templates for energy storage and conversion applications.
引文
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7 Viswanathan V,Thygesen KS,Hummelsh?j JS,et al.Electrical conductivity in Li2O2and its role in determining capacity limitations in non-aqueous Li-O2batteries.J Chem Phys,2011,135:214704
8 Liu Y,He P,Zhou H.Rechargeable solid-state Li-air and Li-Sbatteries:Materials,construction,and challenges.Adv Energy Mater,2018,8:1701602
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13 Shu C,Li B,Zhang B,et al.Hierarchical nitrogen-doped graphene/carbon nanotube composite cathode for lithium-oxygen batteries.ChemSusChem,2015,8:3973-3976
14 Sun B,Huang X,Chen S,et al.Porous graphene nanoarchitectures:an efficient catalyst for low charge-overpotential,long life,and high capacity lithium-oxygen batteries.Nano Lett,2014,14:3145-3152
15 Lu J,Lei Y,Lau KC,et al.A nanostructured cathode architecture for low charge overpotential in lithium-oxygen batteries.Nat Commun,2013,4:2383
16 Franco AA,Xue KH.Carbon-based electrodes for lithium air batteries:Scientific and technological challenges from a modeling perspective.ECS J Solid State Sci Technol,2013,2:M3084-M3100
17 Tran C,Yang XQ,Qu D.Investigation of the gas-diffusionelectrode used as lithium/air cathode in non-aqueous electrolyte and the importance of carbon material porosity.J Power Sources,2010,195:2057-2063
18 Yang X,He P,Xia Y.Preparation of mesocellular carbon foam and its application for lithium/oxygen battery.Electrochem Commun,2009,11:1127-1130
19 Nie H,Zhang H,Zhang Y,et al.Nitrogen enriched mesoporous carbon as a high capacity cathode in lithium-oxygen batteries.Nanoscale,2013,5:8484-8487
20 Kang J,Li OL,Saito N.Hierarchical meso-macro structure porous carbon black as electrode materials in Li-air battery.J Power Sources,2014,261:156-161
21 Xiao J,Mei D,Li X,et al.Hierarchically porous graphene as a lithium-air battery electrode.Nano Lett,2011,11:5071-5078
22 Wang ZL,Xu D,Xu JJ,et al.Graphene oxide gel-derived,freestanding,hierarchically porous carbon for high-capacity and highrate rechargeable Li-O2batteries.Adv Funct Mater,2012,22:3699-3705
23 Lin Y,Moitoso B,Martinez-Martinez C,et al.Ultrahigh-capacity lithium-oxygen batteries enabled by dry-pressed holey graphene air cathodes.Nano Lett,2017,17:3252-3260
24 McCloskey BD,Speidel A,Scheffler R,et al.Twin problems of interfacial carbonate formation in nonaqueous Li-O2batteries.JPhys Chem Lett,2012,3:997-1001
25 Ottakam Thotiyl MM,Freunberger SA,Peng Z,et al.The carbon electrode in nonaqueous Li-O2cells.J Am Chem Soc,2013,135:494-500
26 Yao X,Dong Q,Cheng Q,et al.Why do lithium-oxygen batteries fail:Parasitic chemical reactions and their synergistic effect.Angew Chem Int Ed,2016,55:11344-11353
27 Sun B,Chen S,Liu H,et al.Mesoporous carbon nanocube architecture for high-performance lithium-oxygen batteries.Adv Funct Mater,2015,25:4436-4444
28 Liu Y,Ai K,Lu L.Polydopamine and its derivative materials:Synthesis and promising applications in energy,environmental,and biomedical fields.Chem Rev,2014,114:5057-5115
29 Xiao L,Mei D,Cao M,et al.Effects of structural patterns and degree of crystallinity on the performance of nanostructured ZnOas anode material for lithium-ion batteries.J Alloys Compd,2015,627:455-462
30 Kuo CL,Kuo TJ,Huang MH.Hydrothermal synthesis of ZnOmicrospheres and hexagonal microrods with sheetlike and platelike nanostructures.J Phys Chem B,2005,109:20115-20121
31 Kaneko K.Determination of pore size and pore size distribution.JMembrane Sci,1994,96:59-89
32 Zhang Y,Zhang H,Li J,et al.The use of mixed carbon materials with improved oxygen transport in a lithium-air battery.J Power Sources,2013,240:390-396
33 Horstmann B,Gallant B,Mitchell R,et al.Rate-dependent morphology of Li2O2growth in Li-O2batteries.J Phys Chem Lett,2013,4:4217-4222
34 Kichambare P,Kumar J,Rodrigues S,et al.Electrochemical performance of highly mesoporous nitrogen doped carbon cathode in lithium-oxygen batteries.J Power Sources,2011,196:3310-3316
35 Xie J,Yao X,Cheng Q,et al.Three dimensionally ordered mesoporous carbon as a stable,high-performance Li-O2battery cathode.Angew Chem Int Ed,2015,54:4299-4303
2 Wang L,Zhang Y,Liu Z,et al.Understanding oxygen electrochemistry in aprotic Li-O2batteries.Green Energy Environ,2017,2:186-203
3 Feng N,He P,Zhou H.Critical challenges in rechargeable aprotic Li-O2batteries.Adv Energy Mater,2016,6:1502303
4 Aurbach D,McCloskey BD,Nazar LF,et al.Advances in understanding mechanisms underpinning lithium-air batteries.Nat Energy,2016,1:16128
5 Adams BD,Radtke C,Black R,et al.Current density dependence of peroxide formation in the Li-O2battery and its effect on charge.Energy Environ Sci,2013,6:1772-1778
6 Peng Z,Freunberger SA,Chen Y,et al.A reversible and higherrate Li-O2battery.Science,2012,337:563-566
7 Viswanathan V,Thygesen KS,Hummelsh?j JS,et al.Electrical conductivity in Li2O2and its role in determining capacity limitations in non-aqueous Li-O2batteries.J Chem Phys,2011,135:214704
8 Liu Y,He P,Zhou H.Rechargeable solid-state Li-air and Li-Sbatteries:Materials,construction,and challenges.Adv Energy Mater,2018,8:1701602
9 Song K,Agyeman DA,Jung J,et al.A review of the design strategies for tailored cathode catalyst materials in rechargeable LiO2batteries.Isr J Chem,2015,55:458-471
10 Ma Z,Yuan X,Li L,et al.A review of cathode materials and structures for rechargeable lithium-air batteries.Energy Environ Sci,2015,8:2144-2198
11 Yin YB,Xu JJ,Liu QC,et al.Macroporous interconnected hollow carbon nanofibers inspired by golden-toad eggs toward a binderfree,high-rate,and flexible electrode.Adv Mater,2016,28:7494-7500
12 Guo Z,Zhou D,Dong XL,et al.Ordered hierarchical mesoporous/macroporous carbon:a high-performance catalyst for rechargeable Li-O2batteries.Adv Mater,2013,25:5668-5672
13 Shu C,Li B,Zhang B,et al.Hierarchical nitrogen-doped graphene/carbon nanotube composite cathode for lithium-oxygen batteries.ChemSusChem,2015,8:3973-3976
14 Sun B,Huang X,Chen S,et al.Porous graphene nanoarchitectures:an efficient catalyst for low charge-overpotential,long life,and high capacity lithium-oxygen batteries.Nano Lett,2014,14:3145-3152
15 Lu J,Lei Y,Lau KC,et al.A nanostructured cathode architecture for low charge overpotential in lithium-oxygen batteries.Nat Commun,2013,4:2383
16 Franco AA,Xue KH.Carbon-based electrodes for lithium air batteries:Scientific and technological challenges from a modeling perspective.ECS J Solid State Sci Technol,2013,2:M3084-M3100
17 Tran C,Yang XQ,Qu D.Investigation of the gas-diffusionelectrode used as lithium/air cathode in non-aqueous electrolyte and the importance of carbon material porosity.J Power Sources,2010,195:2057-2063
18 Yang X,He P,Xia Y.Preparation of mesocellular carbon foam and its application for lithium/oxygen battery.Electrochem Commun,2009,11:1127-1130
19 Nie H,Zhang H,Zhang Y,et al.Nitrogen enriched mesoporous carbon as a high capacity cathode in lithium-oxygen batteries.Nanoscale,2013,5:8484-8487
20 Kang J,Li OL,Saito N.Hierarchical meso-macro structure porous carbon black as electrode materials in Li-air battery.J Power Sources,2014,261:156-161
21 Xiao J,Mei D,Li X,et al.Hierarchically porous graphene as a lithium-air battery electrode.Nano Lett,2011,11:5071-5078
22 Wang ZL,Xu D,Xu JJ,et al.Graphene oxide gel-derived,freestanding,hierarchically porous carbon for high-capacity and highrate rechargeable Li-O2batteries.Adv Funct Mater,2012,22:3699-3705
23 Lin Y,Moitoso B,Martinez-Martinez C,et al.Ultrahigh-capacity lithium-oxygen batteries enabled by dry-pressed holey graphene air cathodes.Nano Lett,2017,17:3252-3260
24 McCloskey BD,Speidel A,Scheffler R,et al.Twin problems of interfacial carbonate formation in nonaqueous Li-O2batteries.JPhys Chem Lett,2012,3:997-1001
25 Ottakam Thotiyl MM,Freunberger SA,Peng Z,et al.The carbon electrode in nonaqueous Li-O2cells.J Am Chem Soc,2013,135:494-500
26 Yao X,Dong Q,Cheng Q,et al.Why do lithium-oxygen batteries fail:Parasitic chemical reactions and their synergistic effect.Angew Chem Int Ed,2016,55:11344-11353
27 Sun B,Chen S,Liu H,et al.Mesoporous carbon nanocube architecture for high-performance lithium-oxygen batteries.Adv Funct Mater,2015,25:4436-4444
28 Liu Y,Ai K,Lu L.Polydopamine and its derivative materials:Synthesis and promising applications in energy,environmental,and biomedical fields.Chem Rev,2014,114:5057-5115
29 Xiao L,Mei D,Cao M,et al.Effects of structural patterns and degree of crystallinity on the performance of nanostructured ZnOas anode material for lithium-ion batteries.J Alloys Compd,2015,627:455-462
30 Kuo CL,Kuo TJ,Huang MH.Hydrothermal synthesis of ZnOmicrospheres and hexagonal microrods with sheetlike and platelike nanostructures.J Phys Chem B,2005,109:20115-20121
31 Kaneko K.Determination of pore size and pore size distribution.JMembrane Sci,1994,96:59-89
32 Zhang Y,Zhang H,Li J,et al.The use of mixed carbon materials with improved oxygen transport in a lithium-air battery.J Power Sources,2013,240:390-396
33 Horstmann B,Gallant B,Mitchell R,et al.Rate-dependent morphology of Li2O2growth in Li-O2batteries.J Phys Chem Lett,2013,4:4217-4222
34 Kichambare P,Kumar J,Rodrigues S,et al.Electrochemical performance of highly mesoporous nitrogen doped carbon cathode in lithium-oxygen batteries.J Power Sources,2011,196:3310-3316
35 Xie J,Yao X,Cheng Q,et al.Three dimensionally ordered mesoporous carbon as a stable,high-performance Li-O2battery cathode.Angew Chem Int Ed,2015,54:4299-4303