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1 114 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.
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 1 114 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).
出处
《环境科学》
EI
CAS
CSCD
北大核心
2012年第10期3479-3483,共5页
Environmental Science
基金
国家自然科学基金项目(21077050)
江苏省自然科学基金项目(BK2010051
BK2010378)
科技部国际科技合作项目(2010DFA91910)
教育部长江学者和创新团队发展计划项目(IRT1019)
关键词
有序中孔炭
络合还原法
Pd/CMK-3
电催化氧化
甲酸
ordered mesoporous carbons
complexing reduction
Pd/CMK-3
electrocatalytic oxidation
formic acid