Enhanced Supply of Hydroxyl Species in CeO2-Modified Platinum Catalyst Studied by in Situ ATR-FTIR Spectroscopy

被引:88
作者
Katayama, Yu [1 ]
Okanishi, Takeou [1 ]
Muroyama, Hiroki [1 ]
Matsui, Toshiaki [1 ]
Eguchi, Koichi [1 ]
机构
[1] Kyoto Univ, Grad Sch Engn, Dept Energy & Hydrocarbon Chem, Kyoto 6158510, Japan
来源
ACS CATALYSIS | 2016年 / 6卷 / 03期
关键词
in situ ATR-FTIR; hydroxyl adsorption; electrocatalysis in alkaline solution; cerium oxide; platinum; ALKALINE FUEL-CELLS; CO ELECTROOXIDATION; ELECTROCHEMICAL OXIDATION; AMMONIA ELECTROOXIDATION; INFRARED-SPECTROSCOPY; METHANOL OXIDATION; OXYGEN REDUCTION; PD ELECTRODE; PT-RU; SURFACE;
D O I
10.1021/acscatal.6b00108
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
The recent development of anion exchange membranes (AEMs) has increased the potential of anion exchange membrane fuel cells (AEMFCs). Although highly active electro-catalysts for specific reactions have been successfully developed by placing the most importance on the fuel species, only a few studies have focused on OHad (hydroxyl adsorbed species), which is known to be a common reactive species in alkaline environments. In this study, highly oxophilic CeO2 was selected as a surface modifier for a Pt electrode. We first applied in situ attenuated total reflection Fourier transform infrared (ATR-FTIR) spectroscopy to ionomercoated Pt and CeO2-modified Pt surfaces for clarifying the adsorption behavior of OHad. As a result, a distinct change in adsorption behavior of OHad was confirmed in blank KOH solution. These peculiar characteristics were applicable to various electrochemical oxidation reactions. During the ammonia oxidation reaction, the acceleration of the formation of NOad species was observed in CeO2-modified Pt, suggesting the enhancement of OH adsorption. Furthermore, the degree of activity enhancement by CeO2 addition was investigated for the CO oxidation reaction, methanol oxidation reaction, and ethanol oxidation reaction. Under basic conditions, each of these reactions exhibited distinct activity enhancement. In contrast, under acidic conditions, the promoting effect on these reactions was not observed. These results strongly indicate the potential of our catalyst design strategy and the importance of OHad species as reactive species in alkaline environments.
引用
收藏
页码:2026 / 2034
页数:9
相关论文
共 61 条
[1]   Alkaline direct alcohol fuel cells [J].
Antolini, E. ;
Gonzalez, E. R. .
JOURNAL OF POWER SOURCES, 2010, 195 (11) :3431-3450
[2]   Potential-dependent reorientation of water molecules at an electrode/electrolyte interface studied by surface-enhanced infrared absorption spectroscopy [J].
Ataka, K ;
Yotsuyanagi, T ;
Osawa, M .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (25) :10664-10672
[3]   FT-IR study of CO adsorption on Pt/CeO2:: characterisation and structural rearrangement of small Pt particles [J].
Bazin, P ;
Saur, O ;
Lavalley, JC ;
Daturi, M ;
Blanchard, G .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2005, 7 (01) :187-194
[4]  
BOEHM HP, 1971, DISCUSS FARADAY SOC, P264
[5]   AMMONIA-OXYGEN FUEL CELL [J].
CAIRNS, EJ ;
SIMONS, EL ;
TEVEBAUG.AD .
NATURE, 1968, 217 (5130) :780-&
[6]   Formate, an active intermediate for direct oxidation of methanol on Pt electrode [J].
Chen, YX ;
Miki, A ;
Ye, S ;
Sakai, H ;
Osawa, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2003, 125 (13) :3680-3681
[7]   Towards an ammonia-mediated hydrogen economy? [J].
Christensen, CH ;
Johannessen, T ;
Sorensen, RZ ;
Norskov, JK .
CATALYSIS TODAY, 2006, 111 (1-2) :140-144
[8]   The role of adsorbates in the electrochemical oxidation of ammonia on noble and transition metal electrodes [J].
de Vooys, ACA ;
Koper, MTM ;
van Santen, RA ;
van Veen, JAR .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2001, 506 (02) :127-137
[9]   Mathematical modeling of ammonia electrooxidation kinetics in a Polycrystalline Pt rotating disk electrode [J].
Diaz, Luis A. ;
Botte, Gerardine G. .
ELECTROCHIMICA ACTA, 2015, 179 :519-528
[10]   Alternative energy technologies [J].
Dresselhaus, MS ;
Thomas, IL .
NATURE, 2001, 414 (6861) :332-337