Ag/Au/Pt复合催化剂的制备及其对甲酸的电催化氧化

doi:10.6023/A12030017

化学学报 ›› 2012, Vol. 70 ›› Issue (20): 2149-2154.DOI: 10.6023/A12030017 上一篇下一篇

研究论文

Ag/Au/Pt复合催化剂的制备及其对甲酸的电催化氧化

张强, 姚章权, 周蓉, 杜玉扣, 杨平

苏州大学材料与化学化工学部苏州 215123

投稿日期:2012-03-19 发布日期:2012-09-11
通讯作者: 杜玉扣 E-mail:duyk@suda.edu.cn
基金资助:
项目受国家自然科学基金(Nos. 51073114, 20933007)和江苏省高校优势学科建设工程(PAPD)资助.

Fabrication of Ag/Au/Pt Composite Catalysts and Their Electrocatalytic Oxidation for Formic Acid

Zhang Qiang, Yao Zhangquan, Zhou Rong, Du Yukou, Yang Ping

College of Chemistry and Chemical Engineering, Soochow University, Suzhou 215123

Received:2012-03-19 Published:2012-09-11
Supported by:
Project supported by the National Natural Science Foundation of China (Nos. 51073114, 20933007) and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD).

文章分享

1. Ag/Au/Pt复合催化剂的制备及其对甲酸的电催化氧化.PDF(59KB)

摘要/Abstract

利用化学-电化学方法制备了Ag/Au/Pt复合催化剂. 该催化剂以100 nm左右的Ag颗粒为基底, 以化学方法沉积金再电沉积铂, 这降低了贵金属Au和Pt的用量. 通过SEM, EDX和XRD对样品进行表征, 并测试对甲酸的电催化氧化性能. 研究表明, 当Pt∶Au原子数比小于1∶10时, 主要表现为直接氧化, 在较低的Pt负载量(0.71 μg/cm²)情况下, Ag/Au/Pt复合催化剂对甲酸氧化的直接氧化峰电流密度达到最大. 甲酸的电催化氧化稳定性实验表明, 当Pt载量为0.05 μg时, 相对于最大峰电流密度, 循环伏安扫描第100圈时甲酸氧化的直接氧化峰电流密度仅衰减了2.29%. 同时CO氧化剥离实验表明, 当Pt∶Au＝1∶6时, Ag/Au/Pt复合催化剂对CO氧化峰电势最负, 相对于纯Pt催化剂负移了大约0.13 V, 表明该复合催化剂具有更好的抗CO毒化能力.

关键词: 复合催化剂, 甲酸, 电催化, 直接氧化, CO氧化剥离

Ag/Au/Pt composite catalyst has been fabricated by chemical and electrochemical methods. The catalyst is fabricated by the electrodeposition of 100 nm Ag nanoparticle, then Au is deposited by chemical reduction, and Pt is electrodeposited finally, the quantity of Au and Pt is reduced. The samples have been characterized by scanning electron microscopy (SEM), X-ray energy dispersive spectroscopy (EDX) and X-ray diffraction (XRD) techniques. In addition, the electrocatalytic performance of composite electrode materials is measured by cyclic voltammetry (CV) towards formic acid oxidation. The results demonstrate that the as-prepared Ag/Au/Pt composite catalyst with low Pt loading (0.71 μg/cm²) shows much higher catalytic activity than that of the same amount of pure Pt catalyst towards formic acid electrooxidation, and the current density of direct oxidation for formic acid reaches 4541.42 mA/mg. On the other hand, the content of Pt has a significant influence on formic acid oxidation path. It is found that formic acid electrooxidation on the Ag/Au/Pt composite catalyst mainly follows the direct oxidation path only when the atomic ratio of Pt∶Au is less than 1∶10. The enhanced performance is mainly due to the increase of electrochemical active surface area (EASA) through CVs in H₂SO₄ solution. Moreover, the Ag/Au/Pt composite catalyst exhibits greater poisoning tolerance than that of pure Pt during formic acid electrooxidation, shown in the results of chronoamperometre (CA) measurement. The stability of composite catalyst is evaluated via recording the CV scans of 100 cycles of electrodes towards formic acid oxidation. At the 100th cycle, the current density of Ag/Au/Pt electrode just decreases 2.29%, which is far lower compared with the other electrodes. The CO stripping voltammogram in acid medium is recorded as well. The results show clearly that the CO stripping peak position of composite catalyst shifts negatively compared with that of the pure Pt catalyst in the mass. When the atomic ratio of Pt∶Au is 1∶6.0, the composite catalyst presents lowest peak potential for CO electrooxidation.

Key words: composite catalyst, formic acid, electrocatalysis, direct oxidation, CO stripping

引用此文

张强, 姚章权, 周蓉, 杜玉扣, 杨平. Ag/Au/Pt复合催化剂的制备及其对甲酸的电催化氧化[J]. 化学学报, 2012, 70(20): 2149-2154.

Zhang Qiang, Yao Zhangquan, Zhou Rong, Du Yukou, Yang Ping. Fabrication of Ag/Au/Pt Composite Catalysts and Their Electrocatalytic Oxidation for Formic Acid[J]. Acta Chimica Sinica, 2012, 70(20): 2149-2154.

导出引用 EndNote|Reference Manager|ProCite|BibTeX|RefWorks

分享此文

参考文献

[1] Wen, Z.-H.; Liu, J.; Li, J.-H. Adv. Mater. 2008, 20, 743.

[2] Li, Y.-M.; Tang, L.-H.; Li, J.-H. Electrochem. Commun. 2009, 11, 846.

[3] Wen, Z.-H.; Wang, Q.; Li, J.-H. Adv. Funct. Mater. 2008, 18, 959.

[4] Yu, X.; Pickup, P. G. J. Power Sources 2008, 182, 124.

[5] Rhee, Y. W.; Ha, S. Y.; Masel, R. I. J. Power Sources 2003, 117, 35.

[6] Capon, A.; Parsons, R. J. Electroanal. Chem. 1973, 44, 1.

[7] Wasmus, S; Kuver, A. J. Electroanal. Chem. 1999, 461, 14.

[8] Zhou, K.; Chen, M.; Wang, Z.-B. Chinese Battery Industry 2009, 14, 345. (周锴, 陈锰, 王振波, 电池工业, 2009, 14, 345.)

[9] Gasteiger, H. A.; Markovic, N.; Ross, P. N.; Cairns, J. J. Electrochem. Soc. 1994, 141, 1795.

[10] Arico, A. S.; Creti, P.; Kim, H.; Mantegna, R.; Giordano, N.; Antonucci, V. J. Electrochem. Soc. 1996, 143, 3950.

[11] Abdel, R. M. A.; Khalil, M. W.; Hassan, H. B. J. Appl. Electrochem. 2000, 30, 1151.

[12] Choi, J. H.; Jeong, K. J.; Dong, Y.; Han, J.; Lim, T. H.; Lee, J. S.; Sung ,Y. E. J. Power Sources 2006, 163, 71.

[13] Yu, Y.; Hu, Y.; Liu, X.; Deng, W.; Wang, X. Electrochim. Acta 2009, 54, 3092.

[14] Zhang, H.-M.; Jiang, F.-X.; Zhou, R.; Du, Y.-K.; Yang, P. Int. J. Hydrogen Energy 2011, 36, 15052.

[15] Zhou, R.; Zhang, H.-M.; Du, Y.-K.; Yang, P. Acta Chim. Sinica 2011, 69, 1533. (周蓉, 张红梅, 杜玉扣, 杨平, 化学学报, 2011, 69, 1533.)

[16] Antolini, E.; Cardellini, F. J. Alloys Compd. 2001, 315, 118.

[17] Zhang, H.-M.; Zhou, W.-Q.; Du, Y.-K.; Yang, P.; Wang, C.-Y. Electrochem. Commun. 2010, 12, 882.

[18] Zhao, D.; Xu, B.-Q. Phys. Chem. Chem. Phys. 2006, 8, 5106.

[19] Parsons, R.; VanderNoot, T. J. Electroanal. Chem. 1998, 257, 9.

[20] Weber, M.; Wang, J.-T.; Wasmus, S.; Savinell, R. F. J. Electrochem. Soc. 1996, 143, 158.

[21] Capon, A.; Parsons, R. J. Electroanal. Chem. 1973, 45, 205.

[22] Mrozek, M. F.; Luo, H.; Weaver, M. J. Langmuir 2000, 16, 8463.

[23] Markovic, N. M.; Gasteiger, H. A.; Ross, P. N.; Jiang, X.; Villegas, I.; Weaver, M. J. Electrochim. Acta 1995, 40, 91.

[24] Rice, C.; Ha, S.; Masel, R. I.; Waszczuk, P.; Wieckowski, A.; Barnard, T. J. Power Sources 2002, 111, 83.

[25] Chen, G.-Q.; Li, Y.-H.; Wang, D.; Zheng, L.;You, G.-R. J. Power Sources 2011, 196, 8323.

[26] Sun, S.-G.; Clavilier, J. J. Electroanal. Chem. 1988, 240, 147.

[27] Capon, A.; Parsons, R. J. Electroanal Chem. 1973, 45, 205.

[28] Zhou, X.-C.; Liu, C.-P.; Liao, J.-H.; Lu, T.-H. J. Power Sources 2008, 179, 481.

[29] Arenz, M.; Stamenkovic, V.; Schmidt, T. J.; Wandelt, K.; Ross, P. N.; Markovic, N. M. Phys. Chem. Chem. Phys. 2003, 5, 4242.

[30] Park, I. S.; Lee, K. S.; Choi, J. H.; Park, H. Y.; Sung, Y. E. J. Phys. Chem. 2007, 111, 19126.

[31] Kristian, N.; Yan, Y.; Wang, X. Chem. Commun. 2008, (5), 353.

[32] Wang, S.-Y.; Kristian, N.; Jiang, S.-P.; Wang, X. Electrochem. Commun. 2008, 10, 961.

[33] Zhao, M.-C.; Rice, C.; Masel, R.-I.; Waszczuk, P.; Wieckowski, A. J. Electrochem. Soc. 2004, 151, 131.

[34] Wang, Y.-H.; Zhao, D.; Xu, B.-Q. Chin. J. Catal. 2008, 29, 297.

[35] Obradovic, M. D.; Rogan, J. R.; Babic, B. M.; Tripkocic, A. V.; Gautam, A. R. S.; Radmilovic, V. R. J. Power Sources 2012, 197, 72.

[36] Du, B.-C.; Tong, Y.-Y. J. Phys. Chem. B 2005, 109, 17775.Zhou, W.-Q.; Zhai, C.-Y.; Du, Y.-K.; Xu, J.-K.; Yang, P. Int. J. Hydrogen Energy 2009, 34, 9316.

Ag/Au/Pt复合催化剂的制备及其对甲酸的电催化氧化

Fabrication of Ag/Au/Pt Composite Catalysts and Their Electrocatalytic Oxidation for Formic Acid

PDF

补充材料

可视化

被引次数

摘要/Abstract

引用此文

分享此文

参考文献

相关文章 15

编辑推荐

相关统计

本文评价

[1]	李珊, 路俊欣, 刘杰, 蒋绿齐, 易文斌. 氟烷基亚磺酸钠盐电化学合成α-氟烷基酮[J]. 化学学报, 2024, 82(2): 110-114.
[2]	刘建川, 李翠艳, 刘耀祖, 王钰杰, 方千荣. 高稳定二维联咔唑sp²碳共轭共价有机框架材料用于高效电催化氧还原^★[J]. 化学学报, 2023, 81(8): 884-890.
[3]	杨镇鸿, 干晓娟, 王书哲, 段君元, 翟天佑, 刘友文. 金属性Ni₃N纳米粒子的制备与乙二醇电氧化性能^★[J]. 化学学报, 2023, 81(11): 1471-1477.
[4]	刘春梅, 高燕均, 陈鹏亮. 直接甲酸钠/铁氰化钾微流体燃料电池性能研究[J]. 化学学报, 2022, 80(9): 1256-1263.
[5]	闫绍兵, 焦龙, 何传新, 江海龙. ZIF-67/石墨烯复合物衍生的氮掺杂碳限域Co纳米颗粒用于高效电催化氧还原[J]. 化学学报, 2022, 80(8): 1084-1090.
[6]	何家伟, 焦柳, 程雪怡, 陈光海, 吴强, 王喜章, 杨立军, 胡征. 金属有机框架衍生的空心碳纳米笼的结构调控与锂硫电池性能研究[J]. 化学学报, 2022, 80(7): 896-902.
[7]	蒋银龙, 李国超, 陈青松, 徐忠宁, 林姗姗, 郭国聪. 富晶格位错的多孔铋纳米花高效电还原二氧化碳制甲酸盐^※[J]. 化学学报, 2022, 80(6): 703-707.
[8]	王丹, 封波, 张晓昕, 刘亚楠, 裴燕, 乔明华, 宗保宁. 基于热解ZIF-8的氮掺杂碳电化学氧还原合成过氧化氢催化剂[J]. 化学学报, 2022, 80(6): 772-780.
[9]	应霞薇, 浮建军, 曾敏, 刘文, 张天宇, 沈培康, 张信义. 基于BiOCl-Fe₂O₃@TiO₂介孔复合材料的光电化学合成氨性能研究[J]. 化学学报, 2022, 80(4): 503-509.
[10]	李泽洋, 杨宇森, 卫敏. 二氧化碳还原电催化剂的结构设计及性能研究进展[J]. 化学学报, 2022, 80(2): 199-213.
[11]	安攀, 张庆慧, 杨状, 武佳星, 张佳颖, 王雅君, 李宇明, 姜桂元. 双碳目标下太阳能制氢技术的研究进展[J]. 化学学报, 2022, 80(12): 1629-1642.
[12]	王金格, 周伟, 李佳轶, 丁雅妮, 高继慧. 脉冲电催化的研究进展及性能强化机制[J]. 化学学报, 2022, 80(11): 1555-1568.
[13]	穆春辉, 张艺馨, 寇伟, 徐联宾. 镍氮掺杂有序大孔/介孔碳负载银纳米颗粒用于高效电催化CO₂还原[J]. 化学学报, 2021, 79(7): 925-931.
[14]	马一宁, 施润, 张铁锐. 三相界面电催化二氧化碳还原研究进展[J]. 化学学报, 2021, 79(4): 369-377.
[15]	詹溯, 章福祥. 常温常压电催化合成氨的研究进展[J]. 化学学报, 2021, 79(2): 146-157.