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Mechanistic study of the deactivation of carbon supported Pd during formic acid oxidation
Abstract
Palladium is anattractive anode catalyst for direct formic acid fuel cells (DFAFC) because of its high activity relative to Pt, but it suffers significant activity losses during operation of the DFAFC. The deactivation mechanism of a Pd/C catalyst during oxidation of formic acid has been studied by means of electrochemical stripping voltammetry. The stripping characteristics of the anode poison are virtually the same as those of adsorbed CO, andadsorbed CO has a similar poisoning effect. It is therefore proposed that a gradual build-up of adsorbed CO causes the deactivation of Pd in DFAFCs.
2009 Elsevier B.V. All rights reserved.
1. Introduction
Direct formic acid fuel cell (DFAFC) systems have recently been attracting great attention as promising alternative portable power sources. Pt-based and Pd-based catalysts have been mainly used as anode catalysts for oxidation of the formic acid [1]. The most attractive feature of Pd is its high activity [2,3], which generates much higher power densities than Pt [1]. However, a disadvantage of Pd is that it suffers a serious activity loss over a period of hours under DFAFC conditions [2–5], which has become a significant obstacle for its commercial application.
The electrochemical oxidation of formic acid on Pt is generallyrecognized to follow a ‘dual-pathway’ mechanism [6,7], as described by:
The low activity of Pt is due to rapid poisoning of the surface by adsorbed CO formed in the indirect pathway (Eq. (2)). The higher activity of Pd is thought to be due to dominance of the direct pathway [8,9] and the absence [10] of adsorbed CO on the surface.Although the reason for the slow deactivation of Pd during formic acid oxidation is unknown, it appears to be widely accepted that it is not due to adsorbed CO [10,11]. Formate [9], (bi)sulfate [12], hydroxide [10], and other anions [10] have been proposed as possible adsorbed poisons.
The very long timescale (hours) of the deactivation of Pd DFAFC anodes suggests that the results of mechanistic studies on shorter timescales might provide misleading conclusions. Here we report voltammetric stripping data on Pd/C electrodes that have been deactivated by oxidation of formic acid, and compare the results with those for electrodes that have been poisoned with CO.
2. Experimental
Electrochemical experiments were conducted in a regular 3-electrode electrochemical cell. A Pt wire and Hg/Hg2SO4electrode were used as the counter electrode and the reference electrode,respectively. All potentials are reported relative to Hg/Hg2SO4.The working electrode was prepared by spreading an ink containing 1.28 mg 40% Pd/C catalyst (40% palladium on Vulcan XC-72, ETEK) and 0.32 mg NafionÒonto 1 cm2carbon fiber paper (Toray TGP-H-090). Fluka HPLC grade formic acid (50%, Lot# 09076) was used as the electrolyte together with 0.5 M H2SO4(aq).
5. Conclusion
The poisoning species on Pd/C formed slowly during formic acid oxidation has been ‘isolated’ and electrochemical stripping studies indicate that it is almost certainly adsorbed CO.
Acknowledgements
This work was supported by the Natural Sciences and Engineering Research Council of Canada (NSERC) through a Strategic Projects Grant in partnership with Tekion (Canada) Inc., and by Memorial University.

Answer 1

碳失活的机理研究支持在甲酸氧化钯摘要
钯是直接甲酸燃料电池，因为它的高活性相对于铂（DFAFC中）anattractive阳极催化剂，但它受到的运作期间的重要活动DFAFC中的损失， 期间对甲酸氧化的Pd / C催化剂的失活机理，研究了电化学溶出伏安法。毒药的阳极溶出特性的几乎相同的吸附二氧化碳，一氧化碳andadsorbed也有类似的毒害作用。因此，建议在逐步建立吸附二氧化碳造成的钯DFAFCs停用了。
2009年爱思唯尔BV公司保留所有权利
1。简介：
直接甲酸燃料电池（DFAFC中）系统最近已经吸引了有希望的替代便携式电源的高度重视。铂和钯的基催化剂已被主要用作阳极催化剂对甲酸氧化[1]。钯最吸引人的特点是其高活性[2,3]，从而产生比铂[1]高得多的功率密度。不过，钯的缺点是，它遭受了一小时的条件下DFAFC中时期严重丧失活性[2-5]，这已经成为其商业应用的重大障碍
关于铂甲酸的电化学氧化generallyrecognized遵循'双通道'机制[6,7]，所描述的Pt的活性低，是由于在间接通路形成CO吸附于表面迅速中毒（式（2））。高活性的钯被认为是由于直接通路优势[8,9]以及缺乏对surface.Although [10]在甲酸吸附CO的氧化钯慢失活的原因是未知的，这似乎是人们普遍认为它是不是由于一氧化碳[10,11]。甲酸[9]（双向），硫酸[12]，氢氧化钠[10]等阴离子[10]已被吸附的有毒物质可能提出的。
很长的时间尺度钯DFAFC中的阳极钝化（小时）认为，在更短的时间尺度的机理研究结果可提供误导性的结论。这里，我们报告的Pd / C为已被停用的甲酸氧化电极溶出伏安数据，并与电极用那些已经与一氧化碳中毒的结果
2。实验：
电化学实验是在一定期三电极电化学电池。一个铂丝和Hg/Hg2SO4electrode被用来作为对电极和参比电极分别。 全部潜力相对Hg/Hg2SO4报告。工作电极是由传播含有1.28毫克墨40％的Pd / C催化剂（40火神越野- 72％，钯，ETEK）和0.32毫克NafionÒonto 1 cm2carbon纤维纸（东丽三峡- H型090），Fluka公司色谱纯甲酸（50％，批号09076）被用来作为与0.5 M的硫酸（aq）的电解质在一起。

Answer 2

碳失活的机理研究支持在甲酸氧化钯摘要

1。简介：
直接甲酸燃料电池（DFAFC中）系统最近已经吸引了有希望的替代便携式电源的高度重视。铂和钯的基催化剂已被主要用作阳极催化剂对甲酸氧化[1]。钯最吸引人的特点是其高活性[2,3]，从而产生比铂[1]高得多的功率密度。不过，钯的缺点是，它遭受了一小时的条件下DFAFC中时期严重丧失活性[2-5]，这已经成为其商业应用的重大障碍
关于铂甲酸的电化学氧化generallyrecognized遵循'双通道'机制[6,7]，所描述的Pt的活性低，是由于在间接通路形成CO吸附于表面迅速中毒（式（2））。高活性的钯被认为是由于直接通路优势[8,9]以及缺乏对surface.Although [10]在甲酸吸附CO的氧化钯慢失活的原因是未知的，这似乎是人们普遍认为它是不是由于一氧化碳[10,11]。甲酸[9]（双向），硫酸[12]，氢氧化钠[10]等阴离子[10]已被吸附的有毒物质可能提出的。
很长的时间尺度钯DFAFC中的阳极钝化（小时）认为，在更短的时间尺度的机理研究结果可提供误导性的结论。这里，我们报告的Pd / C已被停用的甲酸氧化电极溶出伏安数据，并与电极用那些已经与一氧化碳中毒的结果
2。实验：
电化学实验是在一定期三电极电化学电池。一个铂丝和Hg/Hg2SO4electrode被用来作为对电极和参比电极分别。 全部潜力相对Hg/Hg2SO4报告。工作电极是由传播含有1.28毫克墨40％的Pd / C催化剂（40火神越野- 72％，钯，ETEK）和0.32毫克NafionÒonto 1 cm2carbon纤维纸（东丽三峡- H型090），Fluka公司色谱纯甲酸（50％，批号09076）被用来作为与0.5 M的硫酸（aq）的电解质在一起。

Answer 3

译：
Mechanistic study of the deactivation of carbon supported Pd during formic acid oxidation
Abstract
Palladium is anattractive anode catalyst for direct formic acid fuel cells (DFAFC) because of its high activity relative to Pt, but it suffers significant activity losses during operation of the DFAFC. The deactivation mechanism of a Pd/C catalyst during oxidation of formic acid has been studied by means of electrochemical stripping voltammetry. The stripping characteristics of the anode poison are virtually the same as those of adsorbed CO, andadsorbed CO has a similar poisoning effect. It is therefore proposed that a gradual build-up of adsorbed CO causes the deactivation of Pd in DFAFCs.
2009 Elsevier B.V. All rights reserved.
1. Introduction
Direct formic acid fuel cell (DFAFC) systems have recently been attracting great attention as promising alternative portable power sources. Pt-based and Pd-based catalysts have been mainly used as anode catalysts for oxidation of the formic acid [1]. The most attractive feature of Pd is its high activity [2,3], which generates much higher power densities than Pt [1]. However, a disadvantage of Pd is that it suffers a serious activity loss over a period of hours under DFAFC conditions [2–5], which has become a significant obstacle for its commercial application.
The electrochemical oxidation of formic acid on Pt is generallyrecognized to follow a ‘dual-pathway’ mechanism [6,7], as described by:
The low activity of Pt is due to rapid poisoning of the surface by adsorbed CO formed in the indirect pathway (Eq. (2)). The higher activity of Pd is thought to be due to dominance of the direct pathway [8,9] and the absence [10] of adsorbed CO on the surface.Although the reason for the slow deactivation of Pd during formic acid oxidation is unknown, it appears to be widely accepted that it is not due to adsorbed CO [10,11]. Formate [9], (bi)sulfate [12], hydroxide [10], and other anions [10] have been proposed as possible adsorbed poisons.
The very long timescale (hours) of the deactivation of Pd DFAFC anodes suggests that the results of mechanistic studies on shorter timescales might provide misleading conclusions. Here we report voltammetric stripping data on Pd/C electrodes that have been deactivated by oxidation of formic acid, and compare the results with those for electrodes that have been poisoned with CO.
2. Experimental
Electrochemical experiments were conducted in a regular 3-electrode electrochemical cell. A Pt wire and Hg/Hg2SO4electrode were used as the counter electrode and the reference electrode,respectively. All potentials are reported relative to Hg/Hg2SO4.The working electrode was prepared by spreading an ink containing 1.28 mg 40% Pd/C catalyst (40% palladium on Vulcan XC-72, ETEK) and 0.32 mg NafionÒonto 1 cm2carbon fiber paper (Toray TGP-H-090). Fluka HPLC grade formic acid (50%, Lot# 09076) was used as the electrolyte together with 0.5 M H2SO4(aq).

Answer 4

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