物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2011年
8期
1868-1874
,共7页
赵静%孙越%李永军%梁韧
趙靜%孫越%李永軍%樑韌
조정%손월%리영군%량인
界面组装%欠电位沉积%Au/Pt复合多层膜%电氧化%甲醇
界麵組裝%欠電位沉積%Au/Pt複閤多層膜%電氧化%甲醇
계면조장%흠전위침적%Au/Pt복합다층막%전양화%갑순
Interfacial self-assembly%Under-potential deposition%Au/Pt composite multilayer film%Electrooxidation%Methanol
采用界面组装、欠电位沉积和氧化还原置换反应组合方法制备了单层Pt/Au复合薄膜,并且不需要任何有机偶联剂;组装单层Pt/Au复合薄膜为三类多层Pt/Au复合薄膜:(Pt/Au)n、Ptm/Au和(Pt3/Au)k(n、m和k分别为Pt/Au、Pt和Pt3/Au的层数).采用电子显微镜研究了Au纳米粒子单层膜和Pt/Au复合多层膜的形貌.对于所有的多层膜电极而言,其电化学活性面积随着层数的增加而增加.通过研究甲醇在每一类Pt/Au复合薄膜上的氧化电流密度,考察了其对甲醇的电催化和抗毒化性能.对于同一类复合薄膜而言,甲醇分别在(Pt/Au)3、Pt3/Au和(Pt3/Au)2电极上均具有最大的氧化电流密度,且优于本体Pt电极.在这三种电极中,(Pt/Au)3电极无论从电流密度上还是从抗毒化能力上讲,其性能是最好的,而且其抗毒化能力也优于商业Pt/C催化剂.这种良好的催化性能源于Au和Pt之间最大化的协同效应,这取决于Pt和Au原子比率以及Pt纳米层和Au纳米层之间的排布方式.
採用界麵組裝、欠電位沉積和氧化還原置換反應組閤方法製備瞭單層Pt/Au複閤薄膜,併且不需要任何有機偶聯劑;組裝單層Pt/Au複閤薄膜為三類多層Pt/Au複閤薄膜:(Pt/Au)n、Ptm/Au和(Pt3/Au)k(n、m和k分彆為Pt/Au、Pt和Pt3/Au的層數).採用電子顯微鏡研究瞭Au納米粒子單層膜和Pt/Au複閤多層膜的形貌.對于所有的多層膜電極而言,其電化學活性麵積隨著層數的增加而增加.通過研究甲醇在每一類Pt/Au複閤薄膜上的氧化電流密度,攷察瞭其對甲醇的電催化和抗毒化性能.對于同一類複閤薄膜而言,甲醇分彆在(Pt/Au)3、Pt3/Au和(Pt3/Au)2電極上均具有最大的氧化電流密度,且優于本體Pt電極.在這三種電極中,(Pt/Au)3電極無論從電流密度上還是從抗毒化能力上講,其性能是最好的,而且其抗毒化能力也優于商業Pt/C催化劑.這種良好的催化性能源于Au和Pt之間最大化的協同效應,這取決于Pt和Au原子比率以及Pt納米層和Au納米層之間的排佈方式.
채용계면조장、흠전위침적화양화환원치환반응조합방법제비료단층Pt/Au복합박막,병차불수요임하유궤우련제;조장단층Pt/Au복합박막위삼류다층Pt/Au복합박막:(Pt/Au)n、Ptm/Au화(Pt3/Au)k(n、m화k분별위Pt/Au、Pt화Pt3/Au적층수).채용전자현미경연구료Au납미입자단층막화Pt/Au복합다층막적형모.대우소유적다층막전겁이언,기전화학활성면적수착층수적증가이증가.통과연구갑순재매일류Pt/Au복합박막상적양화전류밀도,고찰료기대갑순적전최화화항독화성능.대우동일류복합박막이언,갑순분별재(Pt/Au)3、Pt3/Au화(Pt3/Au)2전겁상균구유최대적양화전류밀도,차우우본체Pt전겁.재저삼충전겁중,(Pt/Au)3전겁무론종전류밀도상환시종항독화능력상강,기성능시최호적,이차기항독화능력야우우상업Pt/C최화제.저충량호적최화성능원우Au화Pt지간최대화적협동효응,저취결우Pt화Au원자비솔이급Pt납미층화Au납미층지간적배포방식.
Pt/Au composite monolayer films were fabricated by combining interfacial assembly and under-potential deposition (UPD) with redox replacement.Based on the Pt/Au composite monolayers,an organic linker-free method was proposed for the fabrication of sandwich-like Pt/Au composite multilayer films:(Pt/Au)n,Ptm/Au,and (Pt3/Au)k (n,m,or k represents the layer number).Electron microscopy was used to characterize the morphologies of the Au monolayer films and the Pt/Au composite multilayer films.For each type of composite multilayer films,a common characteristic was that the effective electroactive areas increased with an increase in the layer number.Additionally,the electrocatalytic activities of the composite multilayer films for methanol electrooxidation are systematically discussed by examining the catalytic current densities and its tolerance toward carbonaceous species.For the same series of composite multilayer films (Pt/Au)3,Pt3/Au,and (Pt3/Au)2 showed a higher catalytic current density than bulk Pt (Ptbutk).Among the three composite multilayer films,(Pt/Au)3 showed the best catalytic performance in terms of the current density and tolerance toward carbonaceous species.The tolerance of (Pt/Au)3 to carbonaceous species was found to be better than that of the commercial Pt/C catalyst.This better electrocatalytic activity may be attributed to the maximum synergistic effect between Au and Pt,which depends on the Pt:Au atomic ratio and also the arrangement of Pt and Au nanoparticles.