Chemical vapour deposition of Fe-N-C oxygen reduction catalysts with full utilization of dense Fe-N4 sites

被引：545

作者：

Jiao, Li ^{[1
]}

Li, Jingkun ^{[2
]}

Richard, Lynne LaRochelle ^{[3
]}

Sun, Qiang ^{[3
]}

Stracensky, Thomas ^{[3
]}

Liu, Ershuai ^{[3
]}

Sougrati, Moulay Tahar ^{[2
]}

Zhao, Zipeng ^{[4
]}

Yang, Fan ^{[5
]}

Zhong, Sichen ^{[5
]}

Xu, Hui ^{[5
]}

Mukerjee, Sanjeev ^{[3
]}

Huang, Yu ^{[4
,6
]}

Cullen, David A. ^{[7
]}

Park, Jae Hyung ^{[8
]}

Ferrandon, Magali ^{[8
]}

Myers, Deborah J. ^{[8
]}

Jaouen, Frederic ^{[2
]}

Jia, Qingying ^{[3
]}

机构：

[1] Northeastern Univ, Dept Chem Engn, Boston, MA 02115 USA

[2] Univ Montpellier, Inst Charles Gerhardt Montpellier, CNRS, ENSCM, Montpellier, France

[3] Northeastern Univ, Dept Chem & Chem Biol, Boston, MA 02115 USA

[4] Univ Calif Los Angeles, Dept Mat Sci & Engn, Los Angeles, CA USA

[5] Giner, Newton, MA USA

[6] Univ Calif Los Angeles, Calif NanoSyst Inst, Los Angeles, CA USA

[7] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA

[8] Argonne Natl Lab, Chem Sci & Engn Div, Lemont, IL 60439 USA

来源：

NATURE MATERIALS | 2021年 / 20卷 / 10期

关键词：

FUEL-CELL CATHODES; ACTIVE-SITES; TURNOVER FREQUENCY; IRON; ELECTROCATALYSTS; IDENTIFICATION; ALLOY;

D O I：

10.1038/s41563-021-01030-2

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：

Replacing scarce and expensive platinum (Pt) with metal-nitrogen-carbon (M-N-C) catalysts for the oxygen reduction reaction in proton exchange membrane fuel cells has largely been impeded by the low oxygen reduction reaction activity of M-N-C due to low active site density and site utilization. Herein, we overcome these limits by implementing chemical vapour deposition to synthesize Fe-N-C by flowing iron chloride vapour over a Zn-N-C substrate at 750 degrees C, leading to high-temperature trans-metalation of Zn-N-4 sites into Fe-N-4 sites. Characterization by multiple techniques shows that all Fe-N-4 sites formed via this approach are gas-phase and electrochemically accessible. As a result, the Fe-N-C catalyst has an active site density of 1.92 x 10(20) sites per gram with 100% site utilization. This catalyst delivers an unprecedented oxygen reduction reaction activity of 33 mA cm(-2) at 0.90 V (iR-corrected; i, current; R, resistance) in a H-2-O-2 proton exchange membrane fuel cell at 1.0 bar and 80 degrees C. Replacing platinum with metal-nitrogen-carbon catalysts for the oxygen reduction reaction in proton exchange membrane fuel cells has been impeded by low activity. These limitations have now been overcome by the trans-metalation of Zn-N-4 sites into Fe-N-4 sites.

引用

页码：1385 / +

页数：9

共 51 条

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