Engineering PtRu bimetallic nanoparticles with adjustable alloying degree for methanol electrooxidation: Enhanced catalytic performance

被引:161
作者
Zhang, Junming [1 ]
Qu, Ximing [1 ]
Han, Yu [1 ]
Shen, Linfan [1 ]
Yin, Shuhu [1 ]
Li, Guang [1 ]
Jiang, Yanxia [1 ]
Sun, Shigang [1 ]
机构
[1] Xiamen Univ, Dept Chem, State Key Lab Phys Chem Solid Surfaces, Coll Chem & Chem Engn, Xiamen 361005, Peoples R China
基金
中国国家自然科学基金;
关键词
PtRu alloy; Porous graphitic carbon; Thermal treatment; Methanol oxidation; In-situ FTIRS; OXYGEN REDUCTION REACTION; ONE-POT SYNTHESIS; EFFICIENT CATALYSTS; CARBON NANOTUBES; FACILE SYNTHESIS; ANODE CATALYST; ELECTROCATALYTIC ACTIVITY; ASSISTED SYNTHESIS; HIGHLY EFFICIENT; FUEL-CELL;
D O I
10.1016/j.apcatb.2019.118345
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
PtRu bimetal is of particularly attractive in various electrocatalytic reactions owing to its synergistic effect, ligand effect and strain effect. Here, PtRu nanoalloy supported on porous graphitic carbon (PC) has been successfully prepared via a very facile method involving co-reduction the precursors of Pt and Ru at 300 degrees C by H-2 (PtRu/PC-L) followed by thermal treatment at high temperature (700 degrees C, PtRu/PC-H). Specifically, the electrocatalytic performance of PtRu/PC nanoalloy could be dramatically enhanced through high-temperature annealing. This strategy has synthesized smaller Pt and PtRu nanoparticles (ca. < 3 nm); what's more, they are all homogeneous deposited on the surface of PC. PtRu/PC-H nanocatalyst displays higher alloying degree and stronger electronic interaction between Pt and Ru atoms accompanied by the downshift of Pt d-band center. Studies of electrochemical tests indicate that the as-fabricated PtRu/PC-H sample exhibits superior electrocatalytic performance and excellent CO-poisoning tolerance compared with PtRu/PC-L and Pt/PC nanocatalysts. The mass activity and specific activity on PtRu/PC-H nanoalloy can be increased to 1674.2 mA mg(pt)(-1) and 4.4 mA cm(-2) for MOR, it is 4.08 and 8.80 times higher than that of the Pt/PC nanocatalyst, respectively. From in-situ FTIR spectra, we can discover PtRu/PC-H nanoalloy generates CO2 at a lower potential of -150 mV than those on PtRu/PC-L (0 mV) and Pt/PC (50 mV) nanocatalysts, dramatically improves the ability of cleavage C-H bond and alleviates the CO ads poisoning on active sites. The PtRu/PC-H nanocatalyst exhibits maximum power density of 83.7 mW cm(-2) in single methanol fuel cell test, which more than threefold than that of commercial Pt/C as the anode catalyst. Those experimental results open an effective and clean avenue in the development and preparation of high-performance Pt-based nanocatalysts for direct methanol fuel cells.
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页数:9
相关论文
共 64 条
[1]   Structural and Architectural Evaluation of Bimetallic Nanoparticles: A Case Study of Pt-Ru Core-Shell and Alloy Nanoparticles [J].
Alayoglu, Selim ;
Zavalij, Peter ;
Eichhorn, Bryan ;
Wang, Qi ;
Frenkel, Anatoly I. ;
Chupas, Peter .
ACS NANO, 2009, 3 (10) :3127-3137
[2]   Ruthenium and ruthenium oxide nanofiber supports for enhanced activity of platinum electrocatalysts in the methanol oxidation reaction [J].
An, Geon-Hyoung ;
Lee, Eun-Hwan ;
Ahn, Hyo-Jin .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2016, 18 (22) :14859-14866
[3]  
[Anonymous], ANGEW CHEM INT ED
[4]   Composite anode electrode based on iridium oxide promoter for direct methanol fuel cells [J].
Baglio, V. ;
Sebastian, D. ;
D'Urso, C. ;
Stassi, A. ;
Amin, R. S. ;
El-Khatib, K. M. ;
Arico, A. S. .
ELECTROCHIMICA ACTA, 2014, 128 :304-310
[5]   Performance of vertically oriented graphene supported platinum-ruthenium bimetallic catalyst for methanol oxidation [J].
Bo, Zheng ;
Hu, Dan ;
Kong, Jing ;
Yan, Jianhua ;
Cen, Kefa .
JOURNAL OF POWER SOURCES, 2015, 273 :530-537
[6]   Size-selected synthesis of PtRu nano-catalysts: Reaction and size control mechanism [J].
Bock, C ;
Paquet, C ;
Couillard, M ;
Botton, GA ;
MacDougall, BR .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (25) :8028-8037
[7]   Irrelevance of Carbon Monoxide Poisoning in the Methanol Oxidation Reaction on a PtRu Electrocatalyst [J].
Chen, De-Jun ;
Tong, YuYe J. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2015, 54 (32) :9394-9398
[8]   Electronspun nanofiber network anode for a passive direct methanol fuel cell [J].
Chen, Peng ;
Wu, Huijuan ;
Yuan, Ting ;
Zou, Zhiqing ;
Zhang, Haifeng ;
Zheng, Junwei ;
Yang, Hui .
JOURNAL OF POWER SOURCES, 2014, 255 :70-75
[9]   Effect of operating conditions on the performance of a direct methanol fuel cell with PtRuMo/CNTs as anode catalyst [J].
Chen, Shengzhou ;
Ye, Fei ;
Lin, Weiming .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2010, 35 (15) :8225-8233
[10]   Synthesis of Structurally Ordered Pt3Ti and Pt3V Nanoparticles as Methanol Oxidation Catalysts [J].
Cui, Zhiming ;
Chen, Hao ;
Zhao, Mengtian ;
Marshall, Daniel ;
Yu, Yingchao ;
Abruna, Hector ;
DiSalvo, Francis J. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (29) :10206-10209