Progress in the Development of Fe-Based PGM-Free Electrocatalysts for the Oxygen Reduction Reaction

被引:454
作者
Martinez, Ulises [1 ]
Babu, Siddharth Komini [1 ]
Holby, Edward F. [2 ]
Chung, Hoon T. [1 ]
Yin, Xi [1 ]
Zelenay, Piotr [1 ]
机构
[1] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA
[2] Los Alamos Natl Lab, Sigma Div, Los Alamos, NM 87545 USA
关键词
fuel cells; nonprecious metal electrocatalysts; oxygen reduction reaction (ORR); platinum-group-metal-free (PGM-free) electrocatalysts; DENSITY-FUNCTIONAL THEORY; NITROGEN-DOPED CARBON; METAL-FREE CATHODE; N-C CATALYSTS; MEMBRANE FUEL-CELLS; ACTIVE-SITES; FE/N/C-CATALYSTS; TRANSITION-METALS; ORGANIC FRAMEWORK; ACIDIC MEDIA;
D O I
10.1002/adma.201806545
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Development of alternative energy sources is crucial to tackle challenges encountered by the growing global energy demand. Hydrogen fuel, a promising way to store energy produced from renewable power sources, can be converted into electrical energy at high efficiency via direct electrochemical conversion in fuel cells, releasing water as the sole byproduct. One important drawback to current fuel-cell technology is the high content of platinum-group-metal (PGM) electrocatalysts required to perform the sluggish oxygen reduction reaction (ORR). Addressing this challenge, remarkable progress has been made in the development of low-cost PGM-free electrocatalysts synthesized from inexpensive, earth-abundant, and easily sourced materials such as iron, nitrogen, and carbon (Fe-N-C). PGM-free Fe-N-C electrocatalysts now exhibit ORR activities approaching that of PGM electrocatalysts but at a fraction of the cost, promising to significantly reduce overall fuel-cell technology costs. Herein, recent developments in PGM-free electrocatalysis, demonstrating increased fuel-cell performance, as well as efforts aimed at understanding the key limiting factor, i.e., the nature of the PGM-free active site, are summarized. Further improvements will be accomplished through the controlled and/or rationally designed synthesis of materials with higher active-site densities, while at the same time establishing methods to mitigate catalyst degradation.
引用
收藏
页数:20
相关论文
共 129 条
[51]   A density functional theory study of oxygen reduction reaction on non-PGM Fe-Nx-C electrocatalysts [J].
Kattel, Shyam ;
Atanassov, Plamen ;
Kiefer, Boris .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (27) :13800-13806
[52]   A density functional theory study of oxygen reduction reaction on Me-N4 (Me = Fe, Co, or Ni) clusters between graphitic pores [J].
Kattel, Shyam ;
Wang, Guofeng .
JOURNAL OF MATERIALS CHEMISTRY A, 2013, 1 (36) :10790-10797
[53]   Catalytic activity of Co-Nx/C electrocatalysts for oxygen reduction reaction: a density functional theory study [J].
Kattel, Shyam ;
Atanassov, Plamen ;
Kiefer, Boris .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2013, 15 (01) :148-153
[54]   Density Functional Theory Study of Ni-Nx/C Electrocatalyst for Oxygen Reduction in Alkaline and Acidic Media [J].
Kattel, Shyam ;
Atanassov, Plamen ;
Kiefer, Bons .
JOURNAL OF PHYSICAL CHEMISTRY C, 2012, 116 (33) :17378-17383
[55]   A Combined Probe-Molecule, Mossbauer, Nuclear Resonance Vibrational Spectroscopy, and Density Functional Theory Approach for Evaluation of Potential Iron Active Sites in an Oxygen Reduction Reaction Catalyst [J].
Kneebone, Jared L. ;
Daifuku, Stephanie L. ;
Kehl, Jeffrey A. ;
Wu, Gang ;
Chung, Hoon T. ;
Hu, Michael Y. ;
Alp, E. Ercan ;
More, Karren L. ;
Zelenay, Piotr ;
Holby, Edward F. ;
Neidig, Michael L. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2017, 121 (30) :16283-16290
[56]   Electron knock-on damage in hexagonal boron nitride monolayers [J].
Kotakoski, J. ;
Jin, C. H. ;
Lehtinen, O. ;
Suenaga, K. ;
Krasheninnikov, A. V. .
PHYSICAL REVIEW B, 2010, 82 (11)
[57]   On an Easy Way To Prepare Metal Nitrogen Doped Carbon with Exclusive Presence of MeN4-type Sites Active for the ORR [J].
Kramm, Ulrike I. ;
Herrmann-Geppert, Iris ;
Behrends, Jan ;
Lips, Klaus ;
Fiechter, Sebastian ;
Bogdanoff, Peter .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (02) :635-640
[58]   Correlations between Mass Activity and Physicochemical Properties of Fe/N/C Catalysts for the ORR in PEM Fuel Cell via 57Fe Mossbauer Spectroscopy and Other Techniques [J].
Kramm, Ulrike I. ;
Lefevre, Michel ;
Larouche, Nicholas ;
Schmeisser, Dieter ;
Dodelet, Jean-Pol .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (03) :978-985
[59]   Structure of the catalytic sites in Fe/N/C-catalysts for O2-reduction in PEM fuel cells [J].
Kramm, Ulrike I. ;
Herranz, Juan ;
Larouche, Nicholas ;
Arruda, Thomas M. ;
Lefevre, Michel ;
Jaouen, Frederic ;
Bogdanoff, Peter ;
Fiechter, Sebastian ;
Abs-Wurmbach, Irmgard ;
Mukerjee, Sanjeev ;
Dodelet, Jean-Pol .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2012, 14 (33) :11673-11688
[60]   Stability of carbon nanotubes under electron irradiation: Role of tube diameter and chirality [J].
Krasheninnikov, AV ;
Banhart, F ;
Li, JX ;
Foster, AS ;
Nieminen, RM .
PHYSICAL REVIEW B, 2005, 72 (12)