Fe,N掺杂二维多孔碳双功能催化剂及锌-空气电池中的应用
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摘要
在石墨烯表面负载金属有机框架材料ZIF-8,同时在金属有机框架材料表面分散Fe-2,2-Bipy螯合物,通过高温煅烧分解制备了Fe, N掺杂多孔碳催化剂材料。采用SEM, XRD, XPS对制备的催化剂材料进行了形貌、结构以及成分分析。采用旋转圆盘电极,CV曲线,LSV曲线对Fe,N掺杂多孔碳催化剂材料的氧还原(ORR)以及析氧(OER)电催化性能进行了分析。并且将Fe, N掺杂多孔碳催化剂应用于锌-空气电池。结果表明,所制备的Fe, N掺杂多孔碳催化剂材料显示出均匀的二维结构形貌, Fe元素含量为1.32%。催化剂在0.1 mol/L KOH溶液中半波电位为0.83 V,在1 mol/L KOH溶液中, 10 mA/cm~2电流密度下过电势为420 mV。将催化剂应用于锌-空气电池,锌-空气电池功率密度达到245 mV/cm~2,并且表现出优异的循环稳定性。
Fe, N doped 2D porous carbon catalyst was synthesized by pyrolysizing the precursor, ZIF-8, on graphene. Meanwhile, Fe-2,2-bipy were coordinated on ZIF-8. The catalyst was analyzed by SEM, XRD, and XPS for morphology, structure and component. The ORR and OER performance of the Fe, N doped 2D porous carbon catalyst were characterized by RDE, CV curves and LSV curves. It was found that the Fe, N doped 2 D porous carbon catalyst shows uniform 2D structure and that the content of Fe element is 1.32%. The catalyst shows 0.83 V half-wave potentials for oxygen reduction reaction(ORR) in 0.1 mol/L KOH solution and 420 mV over-potential for oxygen evolution reaction(OER) at 10 m A/cm~2 in 1 mol/L KOH solution. Then, a zinc-air battery was assembled using as-synthesized catalyst. The power density of zinc-air battery is up to 245 mV/cm~2. Furthermore, it shows superior cycling stability.
Fe, N doped 2D porous carbon catalyst was synthesized by pyrolysizing the precursor, ZIF-8, on graphene. Meanwhile, Fe-2,2-bipy were coordinated on ZIF-8. The catalyst was analyzed by SEM, XRD, and XPS for morphology, structure and component. The ORR and OER performance of the Fe, N doped 2D porous carbon catalyst were characterized by RDE, CV curves and LSV curves. It was found that the Fe, N doped 2 D porous carbon catalyst shows uniform 2D structure and that the content of Fe element is 1.32%. The catalyst shows 0.83 V half-wave potentials for oxygen reduction reaction(ORR) in 0.1 mol/L KOH solution and 420 mV over-potential for oxygen evolution reaction(OER) at 10 m A/cm~2 in 1 mol/L KOH solution. Then, a zinc-air battery was assembled using as-synthesized catalyst. The power density of zinc-air battery is up to 245 mV/cm~2. Furthermore, it shows superior cycling stability.
引文
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[2]LI G,WANG X,FU J,et al.Pomegranate-inspired design of highly active and durable bifunctional electrocatalysts for rechargeable metal-air batteries.Angew.Chem.Int.Ed.,2016,55(16):4977-4982.
[3]FU J,LEE D,HASSAN F,et al.Flexible high-energy polymerelectrolyte-based rechargeable zinc-air batteries.Adv.Mater.,2015,27(37):5617-5622.
[4]ABBASI H,SALEHI S,GHORBANI R,et al.Design and manufacturing of a micro zinc-air fuel cell for mobile applications.Iranica J.Energy Environ.,2013,4(2):110-115.
[5]WEI L,KARAHAN H,ZHAI S,et al.Amorphous bimetallic oxidegraphene hybrids as bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries.Adv.Mater.,2017,29(38):1701410-1-10.
[6]ZHANG J,SUN B,ZHAO Y,et al.Modified tetrathiafulvalene as an organic conductor for improving performances of Li-O2 batteries.Angew.Chem.Int.Ed.,2017,56(29):8505-8509.
[7]LIU B,XU W,YAN P,et al.Stabilization of Li metal anode in DMSO-based electrolytes via optimization of salt-solvent coordination for Li-O2 batteries.Adv.Energy Mater.,2017,7(14):1602605-1-10.
[8]HOU Y,HUANG T,WEN Z,et al.Metal-organic frameworkderived nitrogen-doped core-shell-structured porous Fe/Fe3C@Cnanoboxes supported on graphene sheets for efficient oxygen reduction reactions.Adv.Energy Mater.,2014,4(11):1400337-1-8.
[9]NI B,OUYANG C,XU X,et al.Modifying commercial carbon with trace amounts of ZIF to prepare derivatives with superior ORR activities.Adv.Mater.,2017,29(27):1701354-1-7.
[10]LIU J,ZHU D,GUO C,et al.Design strategies toward advanced MOF-derived electrocatalysts for energy-conversion reactions.Adv.Energy Mater.,2017,7(23):1700518-1-26.
[11]YE L,CHAI G,WEN Z.Zn-MOF-74 derived N-doped mesoporous carbon as pH-universal electrocatalyst for oxygen reduction reaction.Adv.Funct.Mater.,2017,27(14):1606190-1-8.
[12]ZHONG H,WANG J,ZHANG Y,et al.ZIF-8 derived graphenebased nitrogen-doped porous carbon sheets as highly efficient and durable oxygen reduction electrocatalysts.Angew.Chem.Int.Ed.,2014,53(51):14235-14239.
[13]CHEN X,LIU B,ZHONG C,et al.Ultrathin Co3O4 layers with large contact area on carbon fibers as high-performance electrode for flexible zinc-air battery integrated with flexible display.Adv.Energy Mater.,2017,7(18):1700779-1-11.
[14]CHEN S,CHENG J,MA L,et al.Light-weight 3D Co-N-doped hollow carbon spheres as efficient electrocatalysts for rechargeable zinc-air batteries.Nanoscale,2018,10(22):10412-10419.
[15]MA L,CHEN S,PEI Z,et al.Single-site active iron-based bifunctional oxygen catalyst for a compressible and rechargeable zinc-air battery.ACS Nano,2018,12(2):1949-1958.
[16]ZAGAI J,KOPER M.Reactivity descriptors for the activity of molecular MN4 catalysts for the oxygen reduction reaction.Angew.Chem.Int.Ed.,2016,55(47):14510-14521.
[17]ZHONG H,WANG J,ZHANG Y,et al.ZIF-8 derived graphenebased nitrogen-doped porous carbon sheets as highly efficient and durable oxygen reduction electrocatalysts.Angew.Chem.Int.Ed.,2014,53(51):14235-14239.
[18]SU C,CHENG H,LI W,et al.Atomic modulation of FeCo-nitrogen-carbon bifunctional oxygen electrodes for rechargeable and flexible all-solid-state zinc-air battery.Adv.Energy Mater.,2017,7(13):1602420-1-12.
[19]LIU K,ZHONG H,MENG F,et al.Recent advances in metal-nitrogen-carbon catalysts for electrochemical water splitting.Mater.Chem.Front.,2017,1(11):2155-2173.
[20]ZHU Y,ZHANG B,LIU X,et al.Unravelling the structure of electrocatalytically active Fe-N complexes in carbon for the oxygen reduction reaction.Angew.Chem.Int.Ed.,2014,53(40):10673-10677.
[21]ZITOLO A,GOELLNER V,ARMEL V,et al.Identification of catalytic sites for oxygen reduction in iron-and nitrogen-doped graphene materials.Nat.Mater.,2015,14(9):937-945.
[22]SHEN H,EDUARDO G,MA J,et al.Synergistic effects between atomically dispersed Fe-N-C and C-S-C for the oxygen reduction reaction in acidic media.Angew.Chem.Int.Ed.,2017,129(44):13988-13992.
[23]MA L,FAN H,FU K,et al.Metal-organic framework/layered carbon nitride nano-sandwiches for superior asymmetric supercapacitor.Chemistry Select,2016,1(13):3730-3738.
[24]MA L,FAN H,WANG J,et al.Water-assisted ions in situ intercalation for porous polymeric graphitic carbon nitride nanosheets with superior photocatalytic hydrogen evolution performance.Appl.Catal.B:Environ.,2016,190:93-102.
[25]MA L,FAN H,FU K,et al.Protonation of g carbon nitride(g-C3N4)for an electrostatically self-assembling carbon@g-C3N4core-shell nanostructure toward high hydrogen evolution.ACSSustain.Chem.Eng.,2017,5(8):7093-7103.
[26]FERRERO G,PREUSS K,MARINOVIC A,et al.Fe-N-doped carbon capsules with outstanding electrochemical performance and stability for the oxygen reduction reaction in both acid and alkaline conditions.ACS Nano,2016,10(6):5922-5932.
[27]JIANG W,GU L,LI L,et al.Understanding the high activity of Fe-N-C electrocatalysts in oxygen reduction:Fe/Fe3C nanoparticles boost the activity of Fe-N-C.J.Am.Chem.Soc.,2016,138(10):3570-3578.
[28]MALKO D,KUCERNAK A,LOPES T.In situ electrochemical quantification of active sites in Fe-N/C non-precious metal catalysts.Nat.Commun.,2016,7:13285-13292.