Effects of the Addition of Antimony, Tin, and Lead to Palladium Catalyst Formulations for the Direct Formic Acid Fuel Cell

被引:76
作者
Haan, John L. [2 ]
Stafford, Kristin M. [2 ]
Masel, Richard I. [1 ]
机构
[1] Univ Illinois, Dept Chem & Biomol Engn, Urbana, IL 61801 USA
[2] Univ Illinois, Dept Chem, Urbana, IL 61801 USA
关键词
NOBLE-METAL ELECTRODES; SPONTANEOUSLY-DEPOSITED PT/PD; AD-ATOMS; ANODIC CATALYST; DIRECT METHANOL; OXIDATION; PLATINUM; PD; ELECTROOXIDATION; ELECTROCATALYSIS;
D O I
10.1021/jp102990t
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
In an operating direct formic acid fuel cell (DFAFC), the palladium catalyst surface poisons and must be periodically regenerated by oxidative stripping. The objective of this paper is to analyze the effects of antimony, tin, and lead additions to the palladium black catalyst that is used in the DFAFC. We discovered that each adatom strongly promotes formic acid oxidation in an electrochemical cell and reduces the amount of CO poison that develops on the catalyst surface after one hour of oxidation, which suggests a steric effect due to the presence of the adatoms. However, after three hours of oxidation, the poisoning is nearly the same with each of the adatoms, which shows the limitations of the steric effect. We also used X-ray photoelectron spectroscopy to demonstrate a shift in the palladium binding energy due to the presence of the adatoms, which suggests an electronic effect is also present. We conclude that the steric and electronic effects cause a significant enhancement to oxidation in an electrochemical cell, although the enhancement is less in an operating fuel cell.
引用
收藏
页码:11665 / 11672
页数:8
相关论文
共 83 条
[1]   CATALYTIC EFFECTS OF MONOLAYERS OF METALS DEPOSITED AT UNDERPOTENTIALS - OXIDATION OF FORMIC-ACID ON PLATINUM [J].
ADZIC, RR ;
SIMIC, DN ;
DRAZIC, DM ;
DESPIC, AR .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1975, 61 (01) :117-120
[2]   ELECTROCATALYSIS BY FOREIGN METAL MONOLAYERS - OXIDATION OF FORMIC-ACID ON PALLADIUM [J].
ADZIC, RR ;
SPASOJEVIC, MD ;
DESPIC, AR .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1978, 92 (01) :31-43
[3]   ELECTROCHEMICAL OXIDATION OF FORMIC-ACID AT NOBLE-METALS - CATALYTIC EFFECTS OF FOREIGN METAL MONOLAYERS [J].
ADZIC, RR ;
SIMIC, DN ;
DESPIC, AR ;
DRAZIC, DM .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1977, 80 (01) :81-99
[4]   ELECTROCATALYSIS BY FOREIGN METAL MONOLAYERS - OXIDATION OF FORMIC-ACID ON PLATINUM [J].
ADZIC, RR ;
SIMIC, DN ;
DESPIC, AR ;
DRAZIC, DM .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1975, 65 (02) :587-601
[5]   Electrochemical adsorption of tin on palladium [J].
Bakos, I ;
Szabó, S .
ELECTROCHIMICA ACTA, 2001, 46 (16) :2507-2513
[6]  
CAPON A, 1973, J ELECTROANAL CHEM, V45, P205, DOI 10.1016/0368-1874(73)85076-2
[7]   OXIDATION OF FORMIC-ACID ON NOBLE-METAL ELECTRODES .2. COMPARISON OF BEHAVIOR OF PURE ELECTRODES [J].
CAPON, A ;
PARSONS, R .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1973, 44 (02) :239-254
[8]   OXIDATION OF FORMIC-ACID AT NOBLE-METAL ELECTRODES .1. REVIEW OF PREVIOUS WORK [J].
CAPON, A ;
PARSONS, R .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1973, 44 (01) :1-7
[9]   Composition effects of FePt alloy nanoparticles on the electro-oxidation of formic acid [J].
Chen, Wei ;
Kim, Jaemin ;
Sun, Shouheng ;
Chen, Shaowei .
LANGMUIR, 2007, 23 (22) :11303-11310
[10]   Study of carbon-supported Au catalyst as the cathodic catalyst in a direct formic acid fuel cell prepared using a polyvinyl alcohol protection method [J].
Chen, Wei ;
Tang, Yawen ;
Bao, Jianchun ;
Gao, Ying ;
Liu, Changpeng ;
Xing, Wei ;
Lu, Tianhong .
JOURNAL OF POWER SOURCES, 2007, 167 (02) :315-318