碳载体预处理对纳米Pt/C电催化性能影响

doi:10.3969/j.issn.0438-1157.2014.11.020

化工学报 ›› 2014, Vol. 65 ›› Issue (11): 4356-4362.DOI: 10.3969/j.issn.0438-1157.2014.11.020

• 催化、动力学与反应器 • 上一篇下一篇

碳载体预处理对纳米Pt/C电催化性能影响

蔡媛融, 黄蕊, 黄龙, 饶路, 陈声培, 周志有, 孙世刚

厦门大学化学化工学院化学系, 固体表面物理化学国家重点实验室, 福建厦门 361005

收稿日期:2014-03-28 修回日期:2014-07-07 出版日期:2014-11-05 发布日期:2014-11-05
通讯作者: 陈声培
基金资助:
国家自然科学基金项目(21373175,21273180).

Effect of pretreatment of carbon support on electrocatalytic properties of Pt/C nanocatalysts

CAI Yuanrong, HUANG Rui, HUANG Long, RAO Lu, CHEN Shengpei, ZHOU Zhiyou, SUN Shigang

State Key Laboratory for Physical Chemistry of Solid Surfaces, Department of Chemistry, School of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China

Received:2014-03-28 Revised:2014-07-07 Online:2014-11-05 Published:2014-11-05
Supported by:
supported by the National Natural Science Foundation of China (21373175, 21273180).

摘要/Abstract

摘要： 利用NaBH₄还原机制,采用经不同方法预处理的碳载体成功制备出Pt/C-HNO₃、Pt/C-H₂O₂和Pt/C 3种碳载铂纳米催化剂.通过扫描电镜(SEM)、透射电镜(HR-TEM)、循环伏安(CV)和CO_ad溶出技术进行表征.结果表明,所制备的催化剂大小分布较为均一,平均粒径约为4 nm;HR-TEM观察发现,Pt/C-HNO₃中铂纳米粒子的表面具有较高的台阶原子密度;在CO_ad溶出实验中Pt/C-HNO₃表现出较强的抗一氧化碳毒化能力;所制备的3种催化剂及商业催化剂Pt/C JM对乙醇氧化的电催化活性顺序为:Pt/C-HNO₃ > Pt/C-H₂O₂ > Pt/C > Pt/C JM,其中Pt/C-HNO₃的电催化活性和稳定性分别为Pt/C JM的1.5倍和1.9倍.

关键词: 催化剂载体, 纳米粒子, 碳载铂, 催化, 乙醇氧化

Abstract: Carbon supported Pt nanocatalysts (Pt/C) are widely used in fuel cells. In this work, three kinds of Pt/C catalysts were successfully prepared via a chemical reduction method by using carbon black pretreated with different methods, i.e., HNO₃-pretreated carbon (Pt/C-HNO₃), H₂O₂-pretreated carbon (Pt/C-H₂O₂) and unpretreated carbon (Pt/C). The morphologies and properties of the as-prepared Pt/C catalysts were characterized by SEM, HR-TEM, CV and CO_adstripping. Pt nanoparticles were dispersed well in these three Pt/C catalysts with average particle size of 3.4, 3.9 and 4.5 nm respectively. HR-TEM observation indicated that Pt/C-HNO₃ possessed high-density of step atoms and CO_ad stripping experiments showed that Pt/C-HNO₃ exhibited the best anti-poisoning property. Comparing the catalytic activities of three as-prepared Pt/C catalysts toward ethanol electrooxidation with commercial Pt/C catalyst (Pt/C JM) showed that the as-prepared catalystsexhibited higher activity and stability than those of Pt/C JM and the order was Pt/C-HNO₃>Pt/C-H₂O₂>Pt/C>Pt/C JM. Especially for Pt/C-HNO₃, its activity and stability were 1.5 times and 1.9 times of those of Pt/C JM respectively.

Key words: catalyst support, nanoparticles, carbon supported platinum, catalysis, ethanol oxidation

中图分类号:

O646

蔡媛融, 黄蕊, 黄龙, 饶路, 陈声培, 周志有, 孙世刚. 碳载体预处理对纳米Pt/C电催化性能影响[J]. 化工学报, 2014, 65(11): 4356-4362.

CAI Yuanrong, HUANG Rui, HUANG Long, RAO Lu, CHEN Shengpei, ZHOU Zhiyou, SUN Shigang. Effect of pretreatment of carbon support on electrocatalytic properties of Pt/C nanocatalysts[J]. CIESC Journal, 2014, 65(11): 4356-4362.

参考文献 28

[1]	Lin L, Zhou C S, Vittayapadung S, Shen X Q, Dong M D. Opportunities and challenges for biodiesel fuel [J]. Applied Energy, 2011, 88 (4): 1020-1031
[2]	Shen Yeye (沈烨烨), Chen Xuelan (陈雪兰), Xie Lei (谢磊), Li Xiulang (李修亮), Wu Yu (吴禹), Zhao Lujun (赵路军). Control of fuel cell air supply system based on LPV model [J]. CIESC Journal (化工学报), 2013, 64 (12): 4529-4535
[3]	Lamy C, Lima A, LeRhun V, Delime F, Coutanceau C, Leger J M. Recent advances in the development of direct alcohol fuel cells (DAFC) [J]. Journal of Power Sources, 2002, 105 (2): 283-296
[4]	Qian Q Y, Yang C, Zhou Y G, Yang S, Xia X H. Efficient C C bond cleavage in ethanol electrooxidation on porous Pt catalysts [J]. Journal of Electroanalytical Chemistry, 2011, 660 (1): 57-63
[5]	Wang Jieying (王洁莹), Chen Shengpei (陈声培), Wang Peng (王鹏), Huang Rui (黄蕊), Li Mingxuan (李明轩), Sun Shigang (孙世刚). Preparation and characterization of carbon supported CoNi alloy nanoparticles electrode and their electrocatalytic properties [J]. CIESC Journal (化工学报), 2010, 61 (S1): 101-105
[6]	Rao Lu (饶路), Jiang Yanxia (姜艳霞), Zhang Binwei (张斌伟), You Lexing (游乐星), Li Zhanhong (李崭虹), Sun Shigang (孙世刚), Electrocatalytic oxidation of ethanol [J]. Progress in Chemistry (化学进展), 2014, 26 (5): 727-736
[7]	Rodríguez-Reinoso F. The role of carbon materials in heterogeneous catalysis [J]. Carbon, 1998, 36 (3): 159-175
[8]	Wilson M H, Garzon F H, Sickafus K E, Gottesfeld S. Surface area loss of supported platinum in polymer electrolyte fuel cells [J]. Journal of the Electrochemical Society, 1993, 140 (10): 2872-2877
[9]	Yu X W, Ye S Y. Recent advances in activity and durability enhancement of Pt/C catalytic cathode in PEMFC (II): Degradation mechanism and durability enhancement of carbon supported platinum catalyst [J]. Journal of Power Sources, 2007, 172 (1): 145-154
[10]	Dicks A L. The role of carbon in fuel cells [J]. Journal of Power Sources, 2006,156 (2): 128-141
[11]	Ross P N, Kinopshita K, Stonehart P. The valence band structure of highly dispersed platinum [J]. Journal of Catalysis, 1974, 32 (1): 163-165
[12]	Kowalczyk Z, Sentek J, Rarog W, Zielinski J, Pielaszek J. Effect of potassium and barium on the stability of a carbon-supported ruthenium catalyst for the synthesis of ammonia [J]. Applied Catalysis A: General, 1998,173 (2): 153-160
[13]	Cameron D S, Cooper S J, Dodgson I L, Harrison B, Jenkins J W. Carbons as supports for precious metal catalysts [J]. Catalysis Today, 1990, 7 (2): 113-137
[14]	Alarcon M C, Valiente A M, Ramos I R, Ruiz A G. Further insights into the Ru nanoparticles-carbon interactions and their role in the catalytic properties [J]. Carbon, 2005, 43 (13): 2711-2722
[15]	Shioyama H, Honjo K, Kiuchi M, Yamada Y, Ueda A, Kuriyama N, Kobayashi T. C2F6 plasma treatment of a carbon support for a PEM fuel cell electrocatalyst [J]. Journal of Power Sources, 2006, 161 (2): 836-838
[16]	Serp P, Corrias M, Kalck P. Carbon nanotubes and nanofibers in catalysis [J]. Applied Catalysis A: General , 2003, 253 (2): 337-358
[17]	Ma J W, Habrioux A, Morais C, Lewera A, Vogel W, Verde-Gomez Y, Ramos-Sanchez G, Balbuena P B, Alonso-Vante N. Spectroelectrochemical probing of the strong interaction between platinum nanoparticles and graphitic domains of carbon [J]. ACS Catalysis, 2013, 3 (9): 1940-1950
[18]	Sebastian D, Suelves I, Pastorb E, Moliner R, Lazaro M J. The effect of carbon nanofiber properties as support for PtRu nanoparticles on the electrooxidation of alcohols [J]. Applied Catalysis B: Environmental, 2013, 132: 13-21
[19]	Sebastian D, Suelves I, Molinera R, Lazaro M J, Stassi A, Bagliob V, Aricob A S. Optimizing the synthesis of carbon nanofiber based electrocatalysts for fuel cells [J]. Applied Catalysis B: Environmental, 2013, 132: 22-27
[20]	Sebastian D, Ruiza A G, Suelves I, Moliner R, Lazaro M J, Baglio V, Stassi A, Arico A S. Enhanced oxygen reduction activity and durability of Pt catalysts supported on carbon nanofibers [J]. Applied Catalysis B: Environmental, 2012, 115: 269-275
[21]	Li W Z, Liang C H, Zhou W J, et al. Preparation and characterization of multiwalled carbon nanotube-supported platinum for cathode catalysts of direct methanol fuel cells [J]. The Journal of Physical Chemistry B, 2003, 107 (26): 6292-6299
[22]	Torres G C, Iablonski E L, Baronetti G T, Castro A A, De Migue S R, Scelza O A, Blanco M D, Pena Jimenez M A, Fierro J L G. Effect of the carbon pre-treatment on the properties and performance for nitrobenzene hydrogenation of Pt/C catalysts [J]. Applied Catalysis A: General, 1997, 161 (1): 213-226
[23]	Maillard F, Schreier S, Hanzlik M, Savinova E R, Weinkauf S, Stimming U. Influence of particle agglomeration on the catalytic activity of carbon-supported Pt nanoparticles in CO monolayer oxidation [J]. Physical Chemistry Chemical Physics, 2005, 7 (2): 385-393
[24]	Lebedeva N P, Koper M T M, Herrero E, Feliu J M, van Santen R A. Cooxidation on stepped Pt [n(111)×(111)] electrodes [J]. Journal of Electroanalytical Chemistry, 2000, 487 (1): 37-44
[25]	Vidal-Iglesias F J, Solla-Gullon J, Campina J M, Herrero E, Aldaz A, Feliu J M. CO monolayer oxidation on stepped Pt (S)[(n-1)(100)×(110)] surfaces [J]. Electrochimica Acta, 2009, 54 (19): 4459-4466
[26]	Lionel Cervera Gontard, Lan-Yun Chang, Crispin J D Hetherington, Angus I Kirkland,Dogan Ozkaya, Rafal E Dunin-Borkowski. Aberration-corrected imaging of active sites on industrial catalyst nanoparticles [J]. Angewandte Chemie, 2007, 119 (20): 3757-3759
[27]	Li N H, Sun S G, Chen S P. Studies on the role of oxidation states of the platinum surface in electrocatalytic oxidation of small primary alcohols [J]. Journal of Electroanalytical Chemistry, 1997, 430 (1/2): 57-67
[28]	Li N H, Sun S G. In situ FTIR spectroscopic studies of electrooxidation of C4 alcohols on platinum electrodes in acid solutions (II): Reaction mechanism of 1,3-butanediol oxidation [J]. Journal of Electroanalytical Chemistry, 1998, 448 (1): 5-15

碳载体预处理对纳米Pt/C电催化性能影响

Effect of pretreatment of carbon support on electrocatalytic properties of Pt/C nanocatalysts

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

参考文献 28

相关文章 15

编辑推荐

Metrics

本文评价

[1]	范孝雄, 郝丽芳, 范垂钢, 李松庚. LaMnO₃/生物炭催化剂低温NH₃-SCR催化脱硝性能研究[J]. 化工学报, 2023, 74(9): 3821-3830.
[2]	李艺彤, 郭航, 陈浩, 叶芳. 催化剂非均匀分布的质子交换膜燃料电池操作条件研究[J]. 化工学报, 2023, 74(9): 3831-3840.
[3]	杨学金, 杨金涛, 宁平, 王访, 宋晓双, 贾丽娟, 冯嘉予. 剧毒气体PH₃的干法净化技术研究进展[J]. 化工学报, 2023, 74(9): 3742-3755.
[4]	吴雷, 刘姣, 李长聪, 周军, 叶干, 刘田田, 朱瑞玉, 张秋利, 宋永辉. 低阶粉煤催化微波热解制备含碳纳米管的高附加值改性兰炭末[J]. 化工学报, 2023, 74(9): 3956-3967.
[5]	程业品, 胡达清, 徐奕莎, 刘华彦, 卢晗锋, 崔国凯. 离子液体基低共熔溶剂在转化CO₂中的应用[J]. 化工学报, 2023, 74(9): 3640-3653.
[6]	陈杰, 林永胜, 肖恺, 杨臣, 邱挺. 胆碱基碱性离子液体催化合成仲丁醇性能研究[J]. 化工学报, 2023, 74(9): 3716-3730.
[7]	杨菲菲, 赵世熙, 周维, 倪中海. Sn掺杂的In₂O₃催化CO₂选择性加氢制甲醇[J]. 化工学报, 2023, 74(8): 3366-3374.
[8]	李凯旋, 谭伟, 张曼玉, 徐志豪, 王旭裕, 纪红兵. 富含零价钴活性位点的钴氮碳/活性炭设计及甲醛催化氧化应用研究[J]. 化工学报, 2023, 74(8): 3342-3352.
[9]	仪显亨, 周骛, 蔡小舒, 蔡天意. 光纤后向动态光散射测量纳米颗粒的浓度适用范围研究[J]. 化工学报, 2023, 74(8): 3320-3328.
[10]	杨欣, 彭啸, 薛凯茹, 苏梦威, 吴燕. 分子印迹-TiO₂光电催化降解增溶PHE废水性能研究[J]. 化工学报, 2023, 74(8): 3564-3571.
[11]	陈雅鑫, 袁航, 刘冠章, 毛磊, 杨纯, 张瑞芳, 张光亚. 蛋白质纳米笼介导的酶自固定化研究进展[J]. 化工学报, 2023, 74(7): 2773-2782.
[12]	汤晓玲, 王嘉瑞, 朱玄烨, 郑仁朝. 基于Pickering乳液的卤醇脱卤酶催化合成手性环氧氯丙烷[J]. 化工学报, 2023, 74(7): 2926-2934.
[13]	余娅洁, 李静茹, 周树锋, 李清彪, 詹国武. 基于天然生物模板构建纳米材料及集成催化剂研究进展[J]. 化工学报, 2023, 74(7): 2735-2752.
[14]	李盼, 马俊洋, 陈志豪, 王丽, 郭耘. Ru/α-MnO₂催化剂形貌对NH₃-SCO反应性能的影响[J]. 化工学报, 2023, 74(7): 2908-2918.
[15]	涂玉明, 邵高燕, 陈健杰, 刘凤, 田世超, 周智勇, 任钟旗. 钙基催化剂的设计合成及应用研究进展[J]. 化工学报, 2023, 74(7): 2717-2734.