Electrocatalytic Properties of N-S-Fe Co-doped HierarchicalPorous Carbon Material Co-Synthesized by Dual-template
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摘要: 通过MgO/ZnCl2双模板协同作用和一步热解的方法制备氮硫铁共掺杂分级多孔碳材料,研究了该材料的氧还原反应电催化性能。结果表明:采用该方法成功合成了具有碳纳米片结构的氮硫铁共掺杂分级多孔碳材料,比表面积较大,为1140.31m2·g-1;ZnCl2模板促进了微孔的形成,有助于形成致密的活性位点;MgO模板促进了介孔的形成,有利于氧还原反应电催化过程的传质;该材料在碱性电解质中表现出优异的氧还原反应电催化活性、良好的电催化稳定性和持久性以及较快的电子转移速率,氧还原反应的起始电位为1.05V,半波电位为0.81V,电荷转移电阻为11Ω·cm2,经过13h极化后保留了原始电流密度的83%;用该材料组装的锌-空气电池的开路电位为1.42V,最大功率密度为182.1mW·cm-2。Abstract: N-S-Fe co-doped hierarchical porous carbon material was prepared by MgO/ZnCl2 double template synergy and one-step pyrolysis, and the electrocatalytic performance of oxygen reduction reaction of the material was studied. The results show that the N-S-Fe co-doped hierarchical porous carbon material with carbon nanosheet structure was successfully synthesized, and had large specific surface area of 1140.31 m2·g-1. The ZnCl2 template could be conducive to the formation of micropores and dense active sites. The MgO template promoted the formation of mesopore, which could be beneficial to the mass transfer during electrocatalytic process of oxygen reduction reaction. The material exhibited excellent oxygen reduction electrocatalytic activity, good electrocatalytic stability and persistence, and high electron transfer rates in alkaline electrolytes. The onset potential, half-wave potential and charge transfer resistance were 1.05 V, 0.81 V and 11 Ω·cm2, respectively. After 13h of polarization, 83% of the original current density was retained. The zinc-air battery assembled with the material had open circuit potential of 1.42 V and maximum power density of 182.1 mW·cm-2.
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[1] LI R,WEI Z D,GOU X L.Nitrogen and phosphorus dual-doped graphene/carbon nanosheets as bifunctional electrocatalysts for oxygen reduction and evolution[J].ACS Catalysis,2015,5(7):4133-4142.
[2] XIANG Q,LIU Y P,ZOU X F,et al.Hydrothermal synthesis of a new kind of N-doped graphene gel-like hybrid as an enhanced ORR electrocatalyst[J].ACS Applied Materials & Interfaces,2018,10(13):10842-10850.
[3] ITO Y,QIU H J,FUJITA T,et al.Bicontinuous nanoporous N-doped graphene for the oxygen reduction reaction[J].Advanced Materials,2014,26(24):4145-4150.
[4] TANG C,WANG H F,CHEN X,et al.Topological defects in metal-free nanocarbon for oxygen electrocatalysis[J].Advanced Materials,2016,28(32):6845-6851.
[5] ZHAO S L,WANG D W,AMAL R,et al.Carbon-based metal-free catalysts for key reactions involved in energy conversion and storage[J].Advanced Materials,2019,31(9):1801526.
[6] LI S C,HU B C,DING Y W,et al.Wood-derived ultrathin carbon nanofiber aerogels[J].Angewandte Chemie,2018,130(24):7203-7208.
[7] CHAO G J,ZHANG L S,WANG D,et al.Activation of graphitic nitrogen sites for boosting oxygen reduction[J].Carbon,2020,159:611-616.
[8] SHI Q,MA Y,QIN L,et al.Metal-free hybrid of nitrogen-doped Nanocarbon@Carbon networks for highly efficient oxygen reduction electrocatalyst[J].ChemElectroChem,2019,6(11):2924-2930.
[9] EISENBERG D,STROEK W,GEELS N J,et al.A simple synthesis of an N-doped carbon ORR catalyst:Hierarchical micro/meso/macro porosity and graphitic shells[J].Chemistry:A European Journal,2016,22(2):501-505.
[10] CHEN L S,CUI X Z,WANG Y X,et al.One-step synthesis of sulfur doped graphene foam for oxygen reduction reactions[J].Dalton Transactions (Cambridge,England:2003),2014,43(9):3420-3423.
[11] LIU J,SONG P,NING Z G,et al.Recent advances in heteroatom-doped metal-free electrocatalysts for highly efficient oxygen reduction reaction[J].Electrocatalysis,2015,6(2):132-147.
[12] LI Q Q,NOFFKE B W,WANG Y L,et al.Electrocatalytic oxygen activation by carbanion intermediates of nitrogen-doped graphitic carbon[J].Journal of the American Chemical Society,2014,136(9):3358-3361.
[13] FANG W G,HU H B,JIANG T T,et al.N-and S-doped porous carbon decorated with in situ synthesized Co-Ni bimetallic sulfides particles:A cathode catalyst of rechargeable Zn-air batteries[J].Carbon,2019,146:476-485.
[14] LIU Y H,YU X Y,FANG Y J,et al.Confining SnS2 ultrathin nanosheets in hollow carbon nanostructures for efficient capacitive sodium storage[J].Joule,2018,2(4):725-735.
[15] CHANG B B,ZHANG S R,SUN L,et al.2D graphene-like hierarchically porous carbon nanosheets from a nano-MgO template and ZnCl2 activation:Morphology,porosity and supercapacitance performance[J].RSC Adv,2016,6(75):71360-71369.
[16] MA Y,CHEN D,FANG Z,et al.High energy density and extremely stable supercapacitors based on carbon aerogels with 100% capacitance retention up to 65,000 cycles[J].PNAS,2021,118(21):e2105610118.
[17] WEI X Q,SONG S J,WU N N,et al.Synergistically enhanced single-atomic site Fe by Fe3C@C for boosted oxygen reduction in neutral electrolyte[J].Nano Energy,2021,84:105840.
[18] ZHANG L, HU Y, JIANG K, et al. The role of sulfur doping in determining the performance of Fe/N-C based electrocatalysts for oxygen reduction reactions[J]. Journal of the Electrochemical Society, 2021, 168(5): 054523.
[19] LIANG H W,WEI W,WU Z S,et al.Mesoporous metal-nitrogen-doped carbon electrocatalysts for highly efficient oxygen reduction reaction[J].Journal of the American Chemical Society,2013,135(43):16002-16005.
[20] SUN Q Y,.Porous carbon material based on biomass prepared by MgO template method and ZnCl2 activation method as electrode for high performance supercapacitor[J].International Journal of Electrochemical Science,2019:1-14.
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