催化学报 ›› 2015, Vol. 36 ›› Issue (7): 943-951.DOI: 10.1016/S1872-2067(15)60863-4

• 论文 • 上一篇    下一篇

聚苯胺对钯催化甲酸电氧化反应的促进作用

马先斌, 冯媛媛, 李扬, 韩运石, 鹿国萍, 杨海芳, 孔德生   

  1. 曲阜师范大学化学与化工学院, 山东省生命有机分析重点实验室, 山东曲阜273165
  • 收稿日期:2015-01-04 修回日期:2015-04-14 出版日期:2015-06-12 发布日期:2015-07-30
  • 通讯作者: 冯媛媛 电话: (0537)4458301; 电子信箱: yfeng@mail.tsinghua.edu.cn
  • 基金资助:

    国家自然科学基金(21403125); 山东省优秀中青年科学家科研奖励基金(BS2011NJ009).

Promoting effect of polyaniline on Pd catalysts for the formic acid electrooxidation reaction

Xianbin Ma, Yuanyuan Feng, Yang Li, Yunshi Han, Guoping Lu, Haifang Yang, Desheng Kong   

  1. Key Laboratory of Life-Organic Analysis, College of Chemistry and Chemical Engineering, Qufu Normal University, Qufu 273165, Shandong, China
  • Received:2015-01-04 Revised:2015-04-14 Online:2015-06-12 Published:2015-07-30
  • Supported by:

    This work is supported by the National Natural Science Foundation of China (21403125) and the Scientific Research Foundation for the Outstanding Young Scientist of Shandong Province (BS2011NJ009).

摘要:

钯基纳米材料是甲酸电氧化反应的优良催化剂. 本工作制备了两个系列钯基催化剂, 并考察了聚苯胺对钯上甲酸电氧化反应的助催化作用. 一种是以聚苯胺为基底, 在其表面电沉积钯纳米粒子, 制得nPANI/Pd催化剂(n表示聚合苯胺的循环数); 另一种是直接在商业Pd/C催化剂表面电聚合苯胺, 制得Pd/C/nPANI催化剂. 结果显示, 聚苯胺单独存在时对甲酸电氧化反应没有催化活性, 但其可对钯上甲酸电氧化反应呈现明显的促进作用, 且促进作用与聚苯胺的厚度(聚合循环数)密切相关. 在两个系列催化剂中, 15PANI/Pd和Pd/C/20PANI显示出最高的催化性能. 15PANI/Pd中钯的质量比催化活性是纯钯催化剂的7.5倍; Pd/C/20PANI中钯的质量比催化活性和本征催化活性分别是商业Pd/C催化剂的2.3和3.3倍. 钯催化性能的提升与聚苯胺和钯纳米粒子间的电子效应有关.

关键词: 钯, 聚苯胺, 电催化, 甲酸电氧化反应

Abstract:

Pd-based nanomaterials have been considered as an effective catalyst for formic acid electrooxidation reaction (FAOR). Herein, we reported two types of polyaniline (PANI)-promoted Pd catalysts. One was an nPANI/Pd electrocatalyst prepared by the electropolymerization of aniline and the electrodeposition of Pd. The other was a Pd/C/nPANI catalyst prepared by the direct electropolymerization of aniline on a commercial Pd/C catalyst. The results show that PANI alone has no catalytic activity for FAOR; however, PANI can exhibit a significant promoting effect to Pd. The current densities of FAOR on the Pd catalysts with a PANI coating show a significant increase compared with that of the Pd reference catalyst without PANI as a promoter. The promoting effects of PANI are strongly dependent on the electropolymerization potential cycles (n). The highest catalytic activities for FAOR of all the nPANI/Pd and Pd/C/nPANI catalysts were those of 15PANI/Pd and Pd/C/20PANI. The mass-specific activity (MSA) of Pd in 15PANI/Pd was 7.5 times that of the Pd catalyst, and the MSA and intrinsic activity of Pd/C/20PANI were 2.3 and 3.3 times that of the Pd/C catalyst, respectively. The enhanced performance of Pd catalysts is proposed as an electronic effect between Pd nanoparticles and PANI.

Key words: Palladium, Polyaniline, Electrocatalysis, Formic acid electrooxidation reaction