Pd/WO3-RGO纳米催化剂对甲酸氧化的电催化性能

doi:10.7503/cjcu20160692

高等学校化学学报 ›› 2017, Vol. 38 ›› Issue (4): 653.doi: 10.7503/cjcu20160692

Pd/WO₃-RGO纳米催化剂对甲酸氧化的电催化性能

金燕仙¹(), 贾文平¹, 梁丹霞¹, 李芳¹, 李嵘嵘¹, 郑梦梦¹, 高为一¹, 倪佳敏¹, 胡佳杰¹, 吴廷华²()

1. 台州学院医药化工学院, 台州 318000
2. 浙江师范大学化学与生命科学学院, 金华 321000

收稿日期:2016-09-29 出版日期:2017-04-10 发布日期:2017-03-23
作者简介:联系人简介: 金燕仙, 女, 博士, 副教授, 主要从事电化学方面的研究. E-mail: snowflakej@163.com;吴廷华, 男, 博士, 教授, 主要从事催化方面的研究. E-mail: thwu@zjut.cn
基金资助:
国家自然科学基金(批准号: 21403150, 21671146, 21506138)、浙江省科技计划项目(批准号: 2014C37052)、浙江省自然科学基金(批准号: LQ15B060001, LQ12B03003)、国家级大学生创新创业训练计划项目(批准号: 201510350013)和台州市科技计划项目(批准号: 1202ky03)资助

Performance of WO₃ Modified Graphene Supported Pd Nanocatalysts for Formic Acid Electro-oxidation^†

JIN Yanxian^1,^*(), JIA Wenping¹, LIANG Danxia¹, LI Fang¹, LI Rongrong¹, ZHENG Mengmeng¹, GAO Weiyi¹, NI Jiamin¹, HU Jiajie¹, WU Tinghua^2,^*()

1. School of Pharmaceutical and Chemical Engineering, Taizhou University, Taizhou 318000, China
2. College of Chemistry and Life Sciences, Zhejiang Normal University, Jinhua 321000, China

Received:2016-09-29 Online:2017-04-10 Published:2017-03-23
Contact: JIN Yanxian,WU Tinghua E-mail:snowflakej@163.com;thwu@zjut.cn
Supported by:
† Supported by the National Natural Science Foundation of China(Nos.21403150, 21671146, 21506138), the Science and Technology Project of Zhejiang Province, China(No.2014C37052), the Zhejiang Provincial Natural Science Foundation, China(Nos LQ15B060001, LQ12B03003), the National Students’ Innovation and Entrepreneurship Training Program of China(No.201510350013) and the Science and Technology Project of Taizhou City, China(No.1202ky03)

摘要/Abstract

摘要：

采用表面修饰技术将WO₃晶粒引入到氧化石墨烯(GO)表面, 通过硼氢化钾还原法制备了载钯催化剂Pd/WO₃-RGO. 对催化剂进行了结构和形貌表征, 并考察了该催化剂对甲酸氧化的电催化性能. 结果表明, Pd/WO₃-RGO催化剂由石墨烯、单斜态WO₃和立方面心Pd晶粒组成, Pd颗粒均匀分散在载体上; 使用Pd/20%WO₃-RGO催化剂电极时的甲酸氧化最大峰电流密度大幅增加, 是Pd/RGO催化剂电极甲酸氧化峰电流密度的2.5倍; Pd/WO₃-RGO催化剂稳定性大大增强, 且具有更加优异的抗CO中毒能力; Pd晶粒与WO₃晶粒的相互交叠有利于它们之间的催化协同效应, 增强催化剂的催化性能.

关键词: 直接甲酸燃料电池, 三氧化钨, 电催化, 石墨烯

Abstract:

The composites WO₃-GO were prepared by the modification of WO₃ crystal particles onto the surface of graphene oxide(GO), Pd/WO₃-RGO catalysts were prepared by using potassium borohydride as the reducing agent. The performances of the catalysts and the effect of different contents of WO₃ on the catalytic activity were investigated. The Pd/WO₃-RGO catalysts showed significantly enhanced electrocatalytic performances for formic acid oxidation. The peak current density on the best catalyst Pd/20%WO₃-RGO catalyst was 2.5 times that on Pd/RGO catalyst. And more importantly, Pd/WO₃-RGO catalysts showed improved stability and excellent tolerance to CO poisoning. According to XRD, TEM and HRTEM results, Pd/WO₃-RGO catalysts are made of monoclinic WO₃, face centered cubic palladium crystal particles and graphene. WO₃ particles are most likely to be covered or overlapped with Pd particles and Pd nanoparticles have a uniform distribution. The enhanced catalytic activity of Pd/WO₃-RGO can be ascribed to the interaction between Pd and WO₃.

Key words: Direct formic acid fuel cell, Tungsten trioxide, Electro-catalysis, Graphene

中图分类号:

O646.5

TrendMD:

金燕仙, 贾文平, 梁丹霞, 李芳, 李嵘嵘, 郑梦梦, 高为一, 倪佳敏, 胡佳杰, 吴廷华. Pd/WO₃-RGO纳米催化剂对甲酸氧化的电催化性能. 高等学校化学学报, 2017, 38(4): 653.

JIN Yanxian, JIA Wenping, LIANG Danxia, LI Fang, LI Rongrong, ZHENG Mengmeng, GAO Weiyi, NI Jiamin, HU Jiajie, WU Tinghua. Performance of WO₃ Modified Graphene Supported Pd Nanocatalysts for Formic Acid Electro-oxidation^†. Chem. J. Chinese Universities, 2017, 38(4): 653.

图/表 6

Fig.1 XRD patterns of Pd/WO3-RGO with different contents of WO3 and Pd/RGO samplesa. GO; b. 10%WO3-GO; c. 20%WO3-GO; d. 30%WO3-GO; e. Pd/10%WO3-RGO; f. Pd/20%WO3-RGO; g. Pd/30%WO3-RGO; h. Pd/RGO.

Fig.2 TEM(A) and HRTEM(B) images, particle size histogram(C) and EDX spectrum(D) of Pd/20%WO3-RGO

Fig.3 Cyclic voltammograms in 0.5 mol/L H2SO4 solution for Pd/WO3-RGO and Pd/RGO electrodesa. Pd/10%WO3-RGO; b. Pd/20%WO3-RGO; c. Pd/30%WO3-RGO; d. Pd/RGO; e. 20%WO3-GO. Scan rate: 50 mV/s.

Fig.4 Cyclic voltammograms in 0.5 mol/L H2SO4+1 mol/L HCOOH solution for Pd/WO3-RGO and Pd/RGO electrodesa. Pd/10%WO3-RGO; b. Pd/20%WO3-RGO; c. Pd/30%WO3-RGO; d. Pd/RGO; e. 20%WO3-GO. f. Pd/15%WO3-RGO; g. Pd/25%WO3-RGO. Scan rate: 50 mV/s.

Fig.5 Chronoamperometric curves at 0.4 V(A) and galvanostatic polarization curves(B) at 4.8 mA/cm2 current density on Pd/WO3-RGO and Pd/RGO electrodes in 0.5 mol/L H2SO4+1 mol/L HCOOH

Fig.6 CO stripping cyclic voltammograms on Pd/20%WO3-RGO(a) and Pd/RGO(b) electrodes in 0.5 mol/L H2SO4 with a scan rate of 50 mV/s

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Pd/WO₃-RGO纳米催化剂对甲酸氧化的电催化性能

Performance of WO₃ Modified Graphene Supported Pd Nanocatalysts for Formic Acid Electro-oxidation^†

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