物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2013年
5期
989-995
,共7页
崔颖§%匡尹杰§%张小华%刘博*%陈金华*
崔穎§%劻尹傑§%張小華%劉博*%陳金華*
최영§%광윤걸§%장소화%류박*%진금화*
Pt纳米颗粒%甲醇%电催化氧化%聚二甲基二烯丙基氯化铵%碳纳米管
Pt納米顆粒%甲醇%電催化氧化%聚二甲基二烯丙基氯化銨%碳納米管
Pt납미과립%갑순%전최화양화%취이갑기이희병기록화안%탄납미관
Pt nanoparticle%Methanol%Electrocatalytic oxidation%PDDA%Carbon nanotube
利用聚二甲基二烯丙基氯化铵(PDDA)非共价修饰的碳纳米管(CNTs)与PtCl62-之间的自发氧化还原作用,制备了Pt纳米颗粒(Pt NPs)/CNTs-PDDA复合催化剂. PDDA在该催化剂中具有三种作用:(1)作为金属前驱体PtCl62-还原为Pt NPs的还原剂;(2)作为原位产生的Pt NPs的稳定剂;(3)在CNTs表面形成保护膜抑制CNTs在甲醇电催化氧化过程中的腐蚀.采用傅里叶变换红外(FTIR)光谱、热重分析和拉曼光谱对CNTs-PDDA进行了表征,表明PDDA通过π-π作用已成功覆盖在CNTs表面,并且修饰过程没有导致CNTs结构的破坏.采用透射电子显微镜(TEM)对Pt NPs/CNTs-PDDA催化剂进行了表征,结果表明, Pt NPs均匀地分散在CNTs上,平均粒径约2 nm,且粒径分布范围窄.用循环伏安法、计时电流法进一步考察了Pt NPs/CNTs-PDDA催化剂在酸性介质中对甲醇的电催化氧化的性能.电化学测试结果表明,与原始CNTs负载的Pt NPs催化剂相比, Pt NPs/CNTs-PDDA催化剂具有更高的电化学活性表面积、电催化质量比活性和稳定性.
利用聚二甲基二烯丙基氯化銨(PDDA)非共價脩飾的碳納米管(CNTs)與PtCl62-之間的自髮氧化還原作用,製備瞭Pt納米顆粒(Pt NPs)/CNTs-PDDA複閤催化劑. PDDA在該催化劑中具有三種作用:(1)作為金屬前驅體PtCl62-還原為Pt NPs的還原劑;(2)作為原位產生的Pt NPs的穩定劑;(3)在CNTs錶麵形成保護膜抑製CNTs在甲醇電催化氧化過程中的腐蝕.採用傅裏葉變換紅外(FTIR)光譜、熱重分析和拉曼光譜對CNTs-PDDA進行瞭錶徵,錶明PDDA通過π-π作用已成功覆蓋在CNTs錶麵,併且脩飾過程沒有導緻CNTs結構的破壞.採用透射電子顯微鏡(TEM)對Pt NPs/CNTs-PDDA催化劑進行瞭錶徵,結果錶明, Pt NPs均勻地分散在CNTs上,平均粒徑約2 nm,且粒徑分佈範圍窄.用循環伏安法、計時電流法進一步攷察瞭Pt NPs/CNTs-PDDA催化劑在痠性介質中對甲醇的電催化氧化的性能.電化學測試結果錶明,與原始CNTs負載的Pt NPs催化劑相比, Pt NPs/CNTs-PDDA催化劑具有更高的電化學活性錶麵積、電催化質量比活性和穩定性.
이용취이갑기이희병기록화안(PDDA)비공개수식적탄납미관(CNTs)여PtCl62-지간적자발양화환원작용,제비료Pt납미과립(Pt NPs)/CNTs-PDDA복합최화제. PDDA재해최화제중구유삼충작용:(1)작위금속전구체PtCl62-환원위Pt NPs적환원제;(2)작위원위산생적Pt NPs적은정제;(3)재CNTs표면형성보호막억제CNTs재갑순전최화양화과정중적부식.채용부리협변환홍외(FTIR)광보、열중분석화랍만광보대CNTs-PDDA진행료표정,표명PDDA통과π-π작용이성공복개재CNTs표면,병차수식과정몰유도치CNTs결구적파배.채용투사전자현미경(TEM)대Pt NPs/CNTs-PDDA최화제진행료표정,결과표명, Pt NPs균균지분산재CNTs상,평균립경약2 nm,차립경분포범위착.용순배복안법、계시전류법진일보고찰료Pt NPs/CNTs-PDDA최화제재산성개질중대갑순적전최화양화적성능.전화학측시결과표명,여원시CNTs부재적Pt NPs최화제상비, Pt NPs/CNTs-PDDA최화제구유경고적전화학활성표면적、전최화질량비활성화은정성.
Carbon nanotubes were non-covalently functionalized by poly(dial yldimethylammonium chloride) (PDDA). Here, PDDA has three roles: reductant for the metal precursor of PtCl62-, stabilizer for in-situ produced Pt nanoparticles (Pt NPs), and anti-corrosion film for carbon nanotubes (CNTs). Surface-functionalization of CNTs with PDDA was characterized by Fourier transform infrared (FTIR) spectrometry, thermogravimetric analysis, and Raman spectroscopy. The results indicated that the surface of CNTs was successful y coated with PDDA film by π-π stacking interactions, and the functionalization process had no detrimental effect on the structure of the CNTs. The obtained catalyst (Pt NPs/CNTs-PDDA) was characterized by transmission electron microscopy, and the results showed that Pt NPs with an average diameter of ca 2 nm were highly dispersed on the surface of CNTs-PDDA. The electrocatalytic properties of Pt NPs/CNTs-PDDA nanohybrids for methanol oxidation were further characterized by cyclic voltammetry and chronoamperometry. Compared with Pt NPs supported on the pristine CNTs, the Pt NPs/CNTs-PDDA catalyst had higher electrochemical surface area and specific mass activity, and better stability towards methanol electro-oxidation.
