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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
引用本文:还中科,宗恩敏,魏丹,万海勤,郑寿荣,许昭怡.Pd/CMK-3的合成、表征及对甲酸的电催化氧化性能研究[J].环境科学,2012,33(10):3479-3483.
作者姓名:还中科  宗恩敏  魏丹  万海勤  郑寿荣  许昭怡
作者单位: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
基金项目: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)
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.

关 键 词:有序中孔炭  络合还原法  Pd/CMK-3  电催化氧化  甲酸
收稿时间:2011/12/29 0:00:00
修稿时间:2012/3/12 0:00:00

Synthesis, Characterization and Electrocatalytic Performance of Pd/CMK-3 for Formic Acid Oxidation
HUAN Zhong-ke,ZONG En-min,WEI Dan,WAN Hai-qin,ZHENG Shou-rong and XU Zhao-yi.Synthesis, Characterization and Electrocatalytic Performance of Pd/CMK-3 for Formic Acid Oxidation[J].Chinese Journal of Environmental Science,2012,33(10):3479-3483.
Authors:HUAN Zhong-ke  ZONG En-min  WEI Dan  WAN Hai-qin  ZHENG Shou-rong and XU Zhao-yi
Institution:State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210046, China;Jiangsu Key Laboratory of Vehicle Emissions Control, Nanjing 210093, China;State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210046, China;Jiangsu Key Laboratory of Vehicle Emissions Control, Nanjing 210093, China;State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210046, China;Jiangsu Key Laboratory of Vehicle Emissions Control, Nanjing 210093, China;State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210046, China;Jiangsu Key Laboratory of Vehicle Emissions Control, Nanjing 210093, China;State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210046, China;Jiangsu Key Laboratory of Vehicle Emissions Control, Nanjing 210093, China;State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210046, China;Jiangsu Key Laboratory of Vehicle Emissions Control, Nanjing 210093, China
Abstract: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).
Keywords:ordered mesoporous carbons  complexing reduction  Pd/CMK-3  electrocatalytic oxidation  formic acid
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