X-ray photoemission spectroscopy analysis of N-containing carbon-based cathode catalysts for polymer electrolyte fuel cells
X-ray photoemission spectroscopy analysis of N-containing carbon-based cathode catalysts for polymer electrolyte fuel cells
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DOI：
10.1016/j.jpowsour.2010.08.054
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发表时间：
2011-02-01
影响因子：
9.2
通讯作者：
Kobayashi, Keisuke
中科院分区：
文献类型：
--
作者：
Niwa, Hideharu;Kobayashi, Masaki;Kobayashi, Keisuke
我们报告了通过硬X射线光电子能谱观察到的用于聚合物电解质燃料电池的三种不同类型的含氮碳基阴极催化剂的电子结构。制备的样品来源于：（1）三聚氰胺和聚（糠醇），（2）氮掺杂炭黑和（3）钴酞菁和酚醛树脂。 C 1s 谱显示了 sp(2) 碳网络形成对于氧还原反应 (ORR) 活性的重要性。碳基阴极催化剂的N 1s 谱被分解为四种组分，分别为类吡啶、类吡咯或类氰化物、类石墨和氧化氮。就氧还原电位而言具有高氧还原反应活性的样品含有高浓度的类石墨氮。不同氧还原反应活性的碳基阴极催化剂的O 1s 谱相似。 ORR 活性和氧含量之间没有相关性。基于对结果的定量分析，碳基阴极催化剂的氧还原反应活性将通过增加发达的sp(2)碳网络中类石墨氮的浓度来提高。 (C) 2010 Elsevier B.V. 保留所有权利。
We report on the electronic structure of three different types of N-containing carbon-based cathode catalysts for polymer electrolyte fuel cells observed by hard X-ray photoemission spectroscopy. Prepared samples are derived from: (1) melamine and poly(furfuryl alcohol), (2) nitrogen-doped carbon black and (3) cobalt phthalocyanine and phenolic resin. C 1s spectra show the importance of sp(2) carbon network formation for the oxygen reduction reaction (ORR) activity. N 1s spectra of the carbon-based cathode catalysts are decomposed into four components identified as pyridine-like, pyrrole- or cyanide-like, graphite-like, and oxide nitrogen. Samples having high oxygen reduction reaction activity in terms of oxygen reduction potential contain high concentration of graphite-like nitrogen. O 1s spectra are similar among carbon-based cathode catalysts of different oxygen reduction reaction activity. There is no correlation between the ORR activity and oxygen content. Based on a quantitative analysis of our results, the oxygen reduction reaction activity of the carbon-based cathode catalysts will be improved by increasing concentration of graphite-like nitrogen in a developed sp(2) carbon network. (C) 2010 Elsevier B.V. All rights reserved.