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Pd/CMK-3的合成、表征及对甲酸的电催化氧化性能研究
摘要点击 2346  全文点击 1116  投稿时间:2011-12-29  修订日期:2012-03-12
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中文关键词  有序中孔炭  络合还原法  Pd/CMK-3  电催化氧化  甲酸
英文关键词  ordered mesoporous carbons  complexing reduction  Pd/CMK-3  electrocatalytic oxidation  formic acid
作者单位E-mail
还中科 南京大学环境学院,污染控制与资源化研究国家重点实验室,南京 210046
江苏省机动车尾气污染控制重点实验室,南京 210093 
hbf87@163.com 
宗恩敏 南京大学环境学院,污染控制与资源化研究国家重点实验室,南京 210046
江苏省机动车尾气污染控制重点实验室,南京 210093 
 
魏丹 南京大学环境学院,污染控制与资源化研究国家重点实验室,南京 210046
江苏省机动车尾气污染控制重点实验室,南京 210093 
 
万海勤 南京大学环境学院,污染控制与资源化研究国家重点实验室,南京 210046
江苏省机动车尾气污染控制重点实验室,南京 210093 
 
郑寿荣 南京大学环境学院,污染控制与资源化研究国家重点实验室,南京 210046
江苏省机动车尾气污染控制重点实验室,南京 210093 
 
许昭怡 南京大学环境学院,污染控制与资源化研究国家重点实验室,南京 210046
江苏省机动车尾气污染控制重点实验室,南京 210093 
zhaoyixu@nju.edu.cn 
中文摘要
      以中孔硅SBA-15为硬模板、蔗糖为炭源,合成了有序中孔炭 CMK-3,并以此CMK-3为载体,采用络合还原法制备了负载量为20%的催化剂Pd/CMK-3. X射线衍射(XRD)和透射电镜(TEM)的结果表明,CMK-3孔结构高度有序,呈现二维六方结构,Pd/CMK-3和Pd/AC(活性炭)催化剂中Pd纳米颗粒分散均匀,平均粒径分别为4.2 nm和4.5 nm; 拉曼光谱测试表明,CMK-3比活性炭的石墨化程度更高,导电性更强; N2吸附/脱附实验表明,CMK-3具有典型的中孔结构,CMK-3的最可几孔径为4.5 nm,显著大于活性炭的0.54 nm,CMK-3的BET比表面积为1114 m2·g-1,大于活性炭的871 m2·g-1. 在对甲酸电催化氧化的循环伏安(CV)和计时电流(CA)测试中,Pd/CMK-3的初始催化活性显著高于Pd/AC,而两者在100 s后的计时电流稳定性则基本相当.
英文摘要
      The synthesis of mesoporous carbons CMK-3 was implemented using SBA-15 samples as the hard templates and sucrose as the carbon source. Ordered mesoporous carbon CMK-3 supported palladium catalyst with a loading amount of 20% (Pd/CMK-3) was prepared by a complexing reduction method. XRD and TEM results showed that the p6mm hexagonal symmetric pore structures of CMK-3 were highly ordered and the Pd nanoparticles with the average size of 4.2 nm and 4.5 nm were well dispersed on CMK-3 and activated carbon (AC) surfaces respectively. Raman results revealed that CMK-3 presented higher graphitization and a higher electric conductivity than AC. The most probable pore size of CMK-3 was 4.5 nm, which is larger than that of AC(0.54 nm). The BET surface area of CMK-3 was 1114 m2·g-1, which was also larger than that of AC(871 m2·g-1). The mesoporous structure of CMK-3 was also observed. The Pd/CMK-3 catalyst exhibited more excellent initial electrocatalytic activity for formic acid oxidation than Pd/AC by cyclic voltammetry (CV). But the chronoamperometry (CA) demonstrated that the stability of the two catalysts were almost equal after 100 s polarization at 0.2 V (vs. SCE).

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