Highly active oxygen reduction non-platinum group metal electrocatalyst without direct metal-nitrogen coordination

被引:606
作者
Strickland, Kara [1 ]
Miner, Elise [1 ]
Jia, Qingying [1 ]
Tylus, Urszula [1 ]
Ramaswamy, Nagappan [1 ]
Liang, Wentao [2 ]
Sougrati, Moulay-Tahar [3 ]
Jaouen, Frederic [3 ]
Mukerjee, Sanjeev [1 ]
机构
[1] Northeastern Univ, Dept Chem & Chem Biol, Ctr Renewable Energy Technol, Egan Res Ctr 317, Boston, MA 02115 USA
[2] Northeastern Univ, Dept Biol, Boston, MA 02115 USA
[3] Inst Charles Gerhardt Montpellier, UMR 5253, F-34095 Montpellier 5, France
来源
NATURE COMMUNICATIONS | 2015年 / 6卷
关键词
HIGH-AREA CARBON; TETRAMETHOXYPHENYL PORPHYRIN; FE/N/C-CATALYSTS; O-2; REDUCTION; IRON; SITES; NANOTUBE; STABILITY; CHLORIDE; DENSITY;
D O I
10.1038/ncomms8343
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Replacement of noble metals in catalysts for cathodic oxygen reduction reaction with transition metals mostly create active sites based on a composite of nitrogen-coordinated transition metal in close concert with non-nitrogen-coordinated carbon-embedded metal atom clusters. Here we report a non-platinum group metal electrocatalyst with an active site devoid of any direct nitrogen coordination to iron that outperforms the benchmark platinumbased catalyst in alkaline media and is comparable to its best contemporaries in acidic media. In situ X-ray absorption spectroscopy in conjunction with ex situ microscopy clearly shows nitrided carbon fibres with embedded iron particles that are not directly involved in the oxygen reduction pathway. Instead, the reaction occurs primarily on the carbon-nitrogen structure in the outer skin of the nitrided carbon fibres. Implications include the potential of creating greater active site density and the potential elimination of any Fenton-type process involving exposed iron ions culminating in peroxide initiated free-radical formation.
引用
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页数:8
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