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̿Ru-Fe߻ֱӼȼϵԭĵ߻о

                    ̿Ru-Fe߻ֱӼȼϵԭĵ߻о
                                               ˬ  ½
    (ʡ﹦ܲصʵңϾʦѧѧ뻷ѧѧԺϾ210097)
    ժҪоΪֱӼȼϵ(DFAFC)߻̿Ru(Ru/C)̿Ru-Fe(Ru-Fe/C)߻ԭĵ߻ܺͿRu-Fe/C߻ԭĵ߻ҪԶRu/C߻һоֻ֣RuγɺϽFeRu/C߻ԭĵ߻ԡ⣬Ru-Fe/C߻Լûе߻ԡˣRu-Fe/C߻ҲкܺõĿԣRu-Fe/C߻ʺΪDFAFC߻
    ؼʣRu/C߻Ru-Fe/C߻ᴦԭ߻
    ͼţO613.71ױʶ룺A±ţ1001-4861(2009)04-0674-05
    𲽷ֱ֣Ӽ״ȼϵ(DMFC)ȣDFAFCкܶŵ[1~6]رǼNafionĤ͸Ҫȼ״2[5]ǻһļᵽ߻ϱͻϵλʹDFAFCܽ͡ˣҪоȶԭиߵ߻־кõĿ߻
    ΪҪڼ״͸ʹDMFC½⣬֮һƶԼ״ûе߻ԺͶԭкõĵ߻ԵPdϴ߻[7]PdԼкܺõĵ߻ԣˣ߻ΪDFAFC߻оڹ籨ʺDFAFCʹõ߻ǶԭнϺõ߻ԶԼûе߻Ե̿Au߲̿Auϴ߻[3,6]Auԭĵ߻Բ̫ߣˣҪһоܸõDFAFC߻
    ӽĤȼϵУȻPtǶԭõĴ߻ǵPtļ۸ϸߣPt;ܹԴȱˣҲйRu߻оRuԭҲнϺõĵ߻ԡңһʹRuϴ߻ʱΪRuױRuһԭĵ߻ԺܵͣҪRu[8,9]DMFCоУҲйRu߻о[10,11]ΪRuԼ״޵߻ԡԭ򣬱оΪDFAFCеRu-Fe/C߻ԭĴ߻ܼ
    1ʵ鲿
    1.1Լ
    Vulcan XC-72̿(Cabot˾)NafionҺ(Aldrichѧ˾ƷNafionΪ5%)ΪԼҺˮơõ߻(THF)H2OĻҺУTHFH2OȾΪ11绯ѧCHI600绯ѧ(CHI˾)ͳ缫ϵĵ绯ѧؽСX-(XRD)D/max-rCתX(ձѧ˾)Уѹ40 kV100mACu KԴΪԴΪ0.154 06 nmʯīɫ˲VantageX(ȵ繫˾)Xɫɢ(EDS)Ϊ5%
    1.2߻Ʊ
    10 mL THF10 mL H2O4.104 mL 0.048 2 molL-1 RuCl3HClҺ0.89 mL 0.062 8 molL-1FeCl3ˮҺϣ30 min80 mg VulcanXC-72̿1 hϾȺ90ˮԡȣҺ10 mL THFH2OҺһŨȵNa2CO3ҺμӵҺеpHֵ9μ10 mLһŨNaBH4H2OTHFҺ1 hʹRuCl3FeCl3ԭȴˮҴĻҺϴӶΣֱCl-Ϊֹ󣬰ѵõĴ߻55ոõĴ߻ΪRu-Fe/C-1߻
    ƵõRu-Fe/C-10.5 molL-1H2SO4Уȵ90棬8 hȴϴӣ55ոõĴ߻ΪRu-Fe/C-2߻
    ƱRu-Fe/C-1߻ƵķƱRu/C߻
    1.3绯ѧ
    绯ѧCHI600绯ѧ(CHI˾)ʿͨAuto-LabתԲ̵缫С绯ѧΪ缫绯ѧأУԵ缫ΪPtƬαȵ缫ΪAg/AgCl缫λAg/AgCl缫ġ缫Ϊ̿缫(ֱ3 mm)ʹǰ6ɰֽ0.30.05mAl2O3׹׹ˮϴӱá10 mg߻0.332mL NafionҺ0.83 mLҴ0.83 mL 3ˮϺ󣬳𵴾ȣȡ2.8Lڲ̿缫棬50ºɣƵù缫Ru-FeΪ10gcm-2
    ڽе绯ѧʱҺΪ0.5 molL-1H2SO4Һ0.5 molL-1 H2SO4+0.5 molL-1HCOOHҺҺ¶ȿ301档ɨʱ缫תΪ2000 rmin-1λɨΪ5 mVs-1ǰͨߴ20 minԳȥҺеڽԭǰͨ20 minʹҺк
    2
    ͼ1Ϊ3ִ߻EDSסͼ1Ru/C߻RuΪ19.6%Ru-Fe/C-1߻RuΪ16.21%FeΪ2.98%RuFeԭӱΪ31ֵRu-Fe/C-2߻УRuΪ14.13%FeΪ0.98%RuFeԭӱԼΪ81EDSһְ붨ķϴˣȿɻȷRuCl3FeCl3϶ԭΣRu-Fe/C-1߻нݺ󣬲Feܽ⡣ǣһFeûܽ⣬ⲿFeRuγ˺Ͻ𣬲ܽ⡣
             
    ͼ2Ϊ3ִ߻XRDͼRu/C߻XRDͼ(ͼ2a)ɼ2Ϊ24.7㴦̼(002)⣬2Ϊ43.0㴦Ru(101)壬Ru/C߻еRuӾṹ(PDF06-0663 Ru)Ru(101)2ֵɼRu3ľֱΪa=b=0.274 46 nmc=0.448 19 nm
           
    Ru-Fe/C-1߻XRDͼ(ͼ2b)УRu101λ43.5㴦Ru/C߻ԴRu-Fe/C߻еRu-FeҲṹвFeRuγɺϽΪFeԭӰ뾶ҪRuСˣFeRuʹ2ֵ侧ֱΪa=b=0.27075 nmc=0.44213 nmҪСRu/C߻Ruľ֤˲FeRuͼ2bɼRu(101)⣬2Ϊ34.653.5㴦2壬ΪFe3O4(324)(408)塣ûй۲쵽Fe壬ûγɺϽFe޶εʽڡ
    Ru-Fe/C-2߻XRDͼ(ͼ2c)еķλRu-Fe/C-1߻ƣϽ𻯵FeСFe3O4ǿȱRu-Fe/C-1߻½ûȫʧFe3O4ûȫܽ⣬ԭ򻹲̫
    ͨScherrerʽ[12]Ru(101)İɼRu/CRu-Fe/C-1Ru-Fe/C-2߻нӵƽֱΪ1.62.11.9 nmڴ߻THFλԭƱģˣӵƽС
    ͼ3ΪRuCl3H2OTHFH2OҺеɨߡͼɼÿУɹ۲쵽2RuCl3Ļԭ壬ӦRu3+ԭRu2+Ru2+ԭRu0ˮҺУRu2+ʼԭλΪ0.25 VTHFH2OҺУRu2+ʼԭλΪ0.30 VˮҺеġͼ4ΪFeCl3H2OTHFH2OҺеɨߡͼɼÿУɹ۲쵽2FeCl3Ļԭ壬ӦFe3+ԭFe2+Fe2+ԭFe0ˮҺУFe2+ʼԭλλ-0.3 V(ͼ4a)THFH2OĻҺУFe2+ʼԭλλ0.07 V(ͼ4b)ˮҺ0.37 VRuCl3FeCl3ںHClˮҺCl-γTHFH2OĻҺУλ̶ȻήͣTHFH2OĻҺRuCl3FeCl3ĻԭλˮҺзơ
             
    ˣˮҺУRu2+Fe2+ʼԭλΪ0.55 VTHFH2OҺУǵʼԭλֻ0.23 VȽϽӽRu2+Fe2+ͬһλͬʱԭˣFe׽ԷγɺϽXRDIJҲƵõRu-Fe/C߻УFeRuľУRuγ˺Ͻ
    ͼ5Ϊͬ߻缫͵H2SO4ҺеɨߡͼɼRu/CRu-Fe/C-1Ru-Fe/C-2߻缫ϣʼԭλֱΪ0.350.440.56 VRu-Fe/C-2߻缫ʼԭλֱRu/CRu-Fe/C-1߻缫0.210.12 V0 VµԭܶȷֱΪ2.63.74.7 mAcm-2ԭĵ߻˳ΪRu-Fe/C-2>Ru-Fe/C-1>Ru/C߻
            
    3ִ߻нӵƽˣֻܹFeRuԭĵ߻ԡRu-Fe/C-1߻нݺ󣬲FeܽõRuγɺϽFeܽ⣬Ruԭĵ߻ҪԴںϽ𻯵FeڽRuFeܸıRuĵܶȣRuԭĵ߻ԡ⣬Ru-Fe/C-1߻УRuγɺϽ⣬һûγɺϽFeFe3O4ָRuĻλ㡣ھᴦ󣬲FeFe3O4ܽ⣬ǵRuλֱ¶ˣRu-Fe/C-2߻ԭĵ߻ԱRu-Fe/C-1߻ߡ
    ͼ6ΪRu-Fe/C-2߻缫͵0.5molL-1 H2SO4Һ0.5 molL-1 H2SO4+0.5 molL-1HCOOHҺеɨߡͼɼ߻ͬͼ6bûгHCOOH[13,14]Ru-Fe/C-2ΪDFAFC߻ʱԼûе߻ԡˣRu-Fe/C-2߻иߵĿ
            
    ͼ7ΪRu-Fe/C-2߻缫͵H2SO4ҺеɨߡͼɼRu-Fe/C-2߻11020ɨ߻غϣ˵ô߻кܺõȶԡ
            
    3
    THFλԭƱDFAFCеRu/CRu-Fe/C߻оǶԭĵ߻ܺͿȷ֣Ru-Fe/C߻ԭĵ߻ҪRu/C߻ΣRu-Fe/C߻ھᴦԭĵ߻ԵõһߡᴦRuγɺϽFeûܽ⣬ˣֻRuγɺϽFeܴٽRu/C߻ԭĵ߻ԡ⣬Ru-Fe/C߻Լûе߻ԣˣᴦRu-Fe/C߻ԭкõĵ߻ԣҲкܺõĿȶԡԣᴦRu-Fe/C߻ʺΪDFAFCе߻
    οף


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