磷钨酸修饰活性炭载Pd催化剂的制备及对甲酸氧化的电催化性能

doi:10.7503/cjcu20130469

高等学校化学学报 ›› 2014, Vol. 35 ›› Issue (1): 115.doi: 10.7503/cjcu20130469

磷钨酸修饰活性炭载Pd催化剂的制备及对甲酸氧化的电催化性能

陆亮¹, 陈婷婷², 葛存旺², 唐亚文¹, 陈煜¹, 陆天虹¹()

1. 江苏省新型动力电池重点实验室, 南京师范大学化学与材料科学学院, 南京 210097
2. 南通大学化学化工学院, 南通 226019

收稿日期:2013-05-17 出版日期:2014-01-10 发布日期:2013-09-13
作者简介:联系人简介: 陆天虹, 男, 博士, 研究员, 博士生导师, 主要从事化学电源研究. E-mail:tianhonglu@263.net
基金资助:
国家自然科学基金(批准号: 21073094, 21273116, 21201105, 61171015)和江苏高校优势学科建设工程项目资助

Preparation of Phosphotungstic Acid-modified Carbon Supported Pd Catalyst and Its Electrocatalytic Performance for Formic Acid Oxidation^†

LU Liang¹, CHEN Tingting², GE Cunwang², TANG Yawen¹, CHEN Yu¹, LU Tianhong^1,^*()

1. Jiangsu Key Laboratory of New Power Batteries, College of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210097, China
2. School of Chemistry and Chemical Engineering, Nantong University, Nantong 226019, China

Received:2013-05-17 Online:2014-01-10 Published:2013-09-13
Contact: LU Tianhong E-mail:tianhonglu@263.net
Supported by:
† Supported by the National Natural Science Foundation of China(Nos.21073094, 21273116, 21201105, 61171015) and Project Funded by the Priority Academic Program Develyment of Jiangsu Higher Education Institutions

摘要/Abstract

摘要：

通过水浴浸泡制备了磷钨酸(PWA)修饰的活性炭(PWA/C), 再通过液相还原法将Pd沉积于PWA/C复合载体上制备了Pd-PWA/C催化剂. 采用X射线能量色散(EDS)谱、 X射线衍射(XRD)谱、透射电子显微镜(TEM)和X射线光电子能谱(XPS)对产物进行表征. 结果表明, 磷钨酸修饰活性炭不仅能有效降低Pd纳米粒子的粒径, 而且与Pd纳米粒子间发生了强烈作用. 电化学测试结果显示, Pd-PWA/C催化剂对甲酸氧化的电催化活性和稳定性均远优于Pd/C催化剂, 这是由于Pd与PWA/C间的强烈作用既能有效降低CO在催化剂上的吸附强度和吸附量, 又能降低甲酸分解的速率, 从而减弱CO的毒化作用.

关键词: 钯催化剂, 磷钨酸, 甲酸氧化, 甲酸分解

Abstract:

Activated carbon was modified with phosphotungstic acid(PWA) at 80 ℃ in a water bath, Pd was then loaded on the PWA/C hybrid support to prepare Pd-PWA/C catalyst by a simple impregnation-reduction method. The measurements of energy dispersive X-ray spectroscopy(EDS), X-ray diffraction(XRD) pattern, transmission electron microscopy(TEM) and X-ray photoelectron spectroscopy(XPS) indicate that phosphotungstic acid-modified carbon not only decreases the average size of Pd nanoparticles effectively but also interacts with Pd nanoparticles strongly. The electrochemical measurements demonstrate that the electrocataly-tic activity and stability of the Pd-PWA/C catalyst for formic acid oxidation are much better than that of the Pd/C catalyst. It is due to that the strong interaction between Pd and PWA/C not only decreases the adsorption strength and amount of CO at the catalyst electrode but also decreases the decomposition rate of formic acid to decrease the CO poisoning.

Key words: Pd catalyst, Phosphotungstic acid, Formic acid oxidation, Decomposition of formic acid

中图分类号:

O646

TrendMD:

陆亮, 陈婷婷, 葛存旺, 唐亚文, 陈煜, 陆天虹. 磷钨酸修饰活性炭载Pd催化剂的制备及对甲酸氧化的电催化性能. 高等学校化学学报, 2014, 35(1): 115.

LU Liang, CHEN Tingting, GE Cunwang, TANG Yawen, CHEN Yu, LU Tianhong. Preparation of Phosphotungstic Acid-modified Carbon Supported Pd Catalyst and Its Electrocatalytic Performance for Formic Acid Oxidation^†. Chem. J. Chinese Universities, 2014, 35(1): 115.

图/表 10

Fig.1 EDS spectra of the PWA/C(A) and Pd-PWA/C(B) catalysts

Fig.2 XRD patterns of the PWA(a), PWA/C(b)(A) and Pd/C(a), Pd-PWA/C(b)(B) catalysts

Fig.3 TEM images(A, C) and corresponding particle size distribution histograms(B, D) of the Pd/C(A, B) and Pd-PWA/C(C, D) catalysts

Fig.4 XPS spectra of Pd3d(A) in the Pd/C(a) and Pd-PWA/C(b) catalysts and W4f(B) in the PWA/C(a) and Pd-PWA/C(b) catalysts

Fig.5 Cyclic voltammograms of 0.5 mol/L H2SO4 solution at the PWA/C(a), Pd/C(b) and Pd-PWA/C(c) catalyst electrodes with a scan rate of 50 mV/s

Fig.6 Cyclic voltammograms of 0.5 mol/L formic acid in 0.5 mol/L H2SO4 solution at the PWA/C(a), Pd/C(b) and Pd-PWA/C(c) catalyst electrodes with a scan rate of 50 mV/s

Fig.7 Chronoamperometric curves of 0.5 mol/L HCOOH in 0.5 mol/L H2SO4 solution at the Pd/C(a) and Pd-PWA/C(b) catalyst electrodes at 0.15 V

Fig.8 Current density vs. cycle numbers curves for the cyclic voltammgrams of 0.5 mol/L HCOOH in 0.5 mol/L H2SO4 solution at the Pd/C(a) and Pd-PWA/C(b) catalyst electrodes with a scan rate of 50 mV/s

Fig.9 Cyclic voltammograms of the adsorbed CO in 0.5 mol/L H2SO4 solution at the Pd/C(a) and Pd-PWA/C(b) catalyst electrodes with a scan rate of 10 mV/s

Fig.10 Relationship between time and the gas vo-lume produced from the catalytic decomposition of HCOOH over the PWA/C(a), Pd-PWA/C(b) and Pd/C(c) catalysts in 0.5 mol/L HCOOH and 0.5 mol/L H2SO4 solution

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磷钨酸修饰活性炭载Pd催化剂的制备及对甲酸氧化的电催化性能

Preparation of Phosphotungstic Acid-modified Carbon Supported Pd Catalyst and Its Electrocatalytic Performance for Formic Acid Oxidation^†

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磷钨酸修饰活性炭载Pd催化剂的制备及对甲酸氧化的电催化性能

Preparation of Phosphotungstic Acid-modified Carbon Supported Pd Catalyst and Its Electrocatalytic Performance for Formic Acid Oxidation†

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Preparation of Phosphotungstic Acid-modified Carbon Supported Pd Catalyst and Its Electrocatalytic Performance for Formic Acid Oxidation^†