Pt/WC-CNTs催化剂的制备及其对氧还原的电催化性能

doi:10.3969/j.issn.0438-1157.2014.10.035

化工学报 ›› 2014, Vol. 65 ›› Issue (10): 4015-4024.DOI: 10.3969/j.issn.0438-1157.2014.10.035

Pt/WC-CNTs催化剂的制备及其对氧还原的电催化性能

金燕仙^1,2, 施梅勤¹, 刘委明¹, 褚有群¹, 徐颖华¹, 马淳安¹, 贾文平², 赵国杰², 余剑清²

1 浙江工业大学化学工程与材料学院, 绿色化学合成技术国家重点实验室培育基地, 科技部能源材料及应用国家国际科技合作基地, 浙江杭州 310032;
2 台州学院医药化工学院, 浙江台州 318000

收稿日期:2014-02-17 修回日期:2014-03-18 出版日期:2014-10-05 发布日期:2014-10-05
通讯作者: 马淳安
基金资助:
科技部国际科技合作重大专项（2010DFB63680）；国家自然科学基金项目（21376220，21106133）；浙江省自然科学基金重点项目（Z4100790）；浙江省自然科学基金青年基金项目（LQ12B03003）；浙江省科技计划项目（2012C37028）。

Pt/WC-CNTs electrocatalyst for oxygen reduction reaction

JIN Yanxian^1,2, SHI Meiqin¹, LIU Weiming¹, CHU Youqun¹, XU Yinghua¹, MA Chun'an¹, JIA Wenping², ZHAO Guojie², YU Jianqing²

1 International Science&Technology Cooperation Base of Energy Materials and Application, Ministry of Science and Technology, State Key Laboratory Breeding Base for Green Chemistry Synthesis Technology, School of Chemical Engineering and Materials Science, Zhejiang University of Technology, Hangzhou 310032, Zhejiang, China;
2 School of Pharmaceutical and Chemical Engineering, Taizhou University, Taizhou 318000, Zhejiang, China)

Received:2014-02-17 Revised:2014-03-18 Online:2014-10-05 Published:2014-10-05
Supported by:
supported by the International Science & Technology Cooperation Program of China (2010DFB63680), the National Natural Science Foundation of China (21376220,21106133), the Natural Science Foundation of Zhejiang Province(Z4100790,LQ12B03003) and Science and Technology Plan Project of Zhejiang Province (2012C37028).

摘要/Abstract

摘要： 通过表面修饰和还原碳化技术制备了以WC为主相的碳化钨/碳纳米管材料（WC-CNTs），并进一步采用微波多元醇法载铂制备复合催化剂Pt/WC-CNTs。该催化剂相比于Pt/CNTs催化剂，具有更低的过电位、更大的电流密度和交换电流密度，且具有更小的电荷转移电阻和更好的氧还原选择性，显示了优异的氧还原电催化性能。XRD结果表明催化剂由多晶面的WC、Pt晶粒和CNTs组成，TEM和HRTEM显示细小的Pt颗粒均匀地分布在WC-CNTs表面。Pt颗粒和WC颗粒紧密接触，这有利于它们之间的催化协同效应，从而大大增强了Pt的氧还原催化活性。旋转圆盘电极研究结果表明Pt/WC-CNTs催化剂对氧还原反应为直接四电子过程。碳化钨/碳纳米管载铂催化剂性能优异、成本较低，在燃料电池阴极催化剂的研究应用中具有良好的发展前景。

关键词: 燃料电池, 电化学, 复合材料, 氧还原, 碳纳米管, 碳化钨

Abstract: Tungsten carbide/carbon nanotubes composite (WC-CNTs) was prepared through surface decoration and in situ reduction and carbonization technology. Furthermore, its supported Pt electrocatalyst was prepared by the microwave-assisted polyol method. Compared to Pt/CNTs catalyst, Pt/WC-CNTs catalyst showed higher electrocatalytic activities for the oxygen reduction reaction (ORR), with lower overpotential, higher current density and higher exchange current density, lower charge transfer resistance and better selectivity towards ORR. XRD and TEM results indicated that Pt/WC-CNTs catalyst was mainly made of WC, Pt and CNTs. Fine Pt particles were dispersed on outside surfaces of WC-CNTs. Pt nanoparticles were in contact with WC nanopaticles, which was helpful to the synergistic effect between them. Thus, the enhancement in electrocatalytic properties of the novel Pt/WC-CNTs catalyst was attributed to this synergistic effect between Pt and WC. The rotating disk electrode measurements were performed to gain insight into ORR performance on Pt/WC-CNTs catalyst. This observation suggested that a four-electron reduction process took place on the catalyst surfaces. Tungsten carbide/carbon nanotube supported Pt electrocatalysts with low cost and unique activity for ORR have good prospect for development in the fuel cell cathode catalyst research applications.

Key words: fuel cells, electrochemistry, composites, oxygen reduction reaction, carbon nanotubes, tungsten carbide

中图分类号:

O646.541

金燕仙, 施梅勤, 刘委明, 褚有群, 徐颖华, 马淳安, 贾文平, 赵国杰, 余剑清. Pt/WC-CNTs催化剂的制备及其对氧还原的电催化性能[J]. 化工学报, 2014, 65(10): 4015-4024.

JIN Yanxian, SHI Meiqin, LIU Weiming, CHU Youqun, XU Yinghua, MA Chun'an, JIA Wenping, ZHAO Guojie, YU Jianqing. Pt/WC-CNTs electrocatalyst for oxygen reduction reaction[J]. CIESC Journal, 2014, 65(10): 4015-4024.

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Pt/WC-CNTs催化剂的制备及其对氧还原的电催化性能

Pt/WC-CNTs electrocatalyst for oxygen reduction reaction

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