Influence of phosphoric anions on oxygen reduction reaction activity of platinum, and strategies to inhibit phosphoric anion adsorption
文献类型：期刊论文
| 作者 | Li, Yuping1,2; Jiang, Luhua1; Wang, Suli1; Sun, Gongquan1 |
| 刊名 | CHINESE JOURNAL OF CATALYSIS
 |
| 出版日期 | 2016-07-01 |
| 卷号 | 37期号:7页码:1134-1141 |
| 关键词 | Platinum Phosphoric Anion Poisoning Oxygen Reduction Reaction Modified Electrode H3po4-pbi Based Fuel Cells |
| ISSN号 | 0253-9837 |
| DOI | 10.1016/S1872-2067(16)62472-5 |
| 文献子类 | Article |
| 英文摘要 | Nafion-membrane-based proton exchange fuel cells (PEMFCs) typically operate at below 100 degrees C. However, H3PO4-doped polybenzimidazole (PBI)-based PEMFCs can operate at 100-200 degrees C. This is advantageous because of accelerated reaction rates and enhanced tolerance to poisons such as CO and SO2, which can arise from reformed gas or the atmosphere. However, the strong adsorption of phosphoric anions on the Pt surface dramatically decreases the electrocatalytic activity. This study exploits the "third-body effect", in which a small amount of organic molecules are pre-adsorbed on the Pt surface to inhibit the adsorption of phosphoric anions. Pre-adsorbate species inhibit the adsorption of phosphoric anions, but can also partially occlude active sites. Thus, the optimum pre-adsorbate coverage is studied by correlating the oxygen reduction reaction (ORR) activity of Pt with pre-adsorbate coverage on the Pt surface. The influence of the pre-adsorbate molecule length is investigated using the organic amines, butylamine, octylamine, and dodecylamine, in both 0.1 mol/L HClO4 and 0.1 mol/L H3PO4. Such amines readily bond to the Pt surface. In aqueous HClO4 electrolyte, the ORR activity of Pt decreases monotonically with increasing pre-adsorbate coverage. In aqueous H3PO4 electrolyte, the ORR activity of Pt initially increases and then decreases with increasing pre-adsorbate coverage. The maximum ORR activity in H3PO4 occurs at a pre-adsorbate coverage of around 20%. The effect of molecular length of the pre-adsorbate is negligible, but its coverage strongly affects the degree to which phosphoric anion adsorption is inhibited. Butylamine adsorbs to Pt at partial active sites, which decreases the electrochemically active surface area. Adsorbed butylamine may also modify the electronic structure of the Pt surface. The ORR activity in the phosphoric acid electrolyte remains relatively low, even when using the pre-adsorbate modified Pt/C catalysts. Further development of the catalyst and electrolyte is required before the commercialization of H3PO4-PBI-based PEMFCs can be realized. (C) 2016, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved. |
| WOS关键词 | POLYMER ELECTROLYTE MEMBRANES ; FUEL-CELLS ; PROTOGENIC GROUP ; ELECTROCATALYTIC ACTIVITY ; INTERMEDIATE TEMPERATURE ; POLYCRYSTALLINE PLATINUM ; SINGLE-CRYSTALS ; MODEL COMPOUNDS ; SULFONIC-ACID ; NANOPARTICLES |
| WOS研究方向 | Chemistry ; Engineering |
| 语种 | 英语 |
| WOS记录号 | WOS:000378972100019 |
| 出版者 | SCIENCE PRESS |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/170450]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 通讯作者 | Jiang, Luhua; Sun, Gongquan |
| 作者单位 | 1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Liaoning, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China |
| 推荐引用方式 GB/T 7714 | Li, Yuping,Jiang, Luhua,Wang, Suli,et al. Influence of phosphoric anions on oxygen reduction reaction activity of platinum, and strategies to inhibit phosphoric anion adsorption[J]. CHINESE JOURNAL OF CATALYSIS,2016,37(7):1134-1141. |
| APA | Li, Yuping,Jiang, Luhua,Wang, Suli,&Sun, Gongquan.(2016).Influence of phosphoric anions on oxygen reduction reaction activity of platinum, and strategies to inhibit phosphoric anion adsorption.CHINESE JOURNAL OF CATALYSIS,37(7),1134-1141. |
| MLA | Li, Yuping,et al."Influence of phosphoric anions on oxygen reduction reaction activity of platinum, and strategies to inhibit phosphoric anion adsorption".CHINESE JOURNAL OF CATALYSIS 37.7(2016):1134-1141. |
入库方式： OAI收割
来源：大连化学物理研究所
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