气候变化领域集成服务门户(CCPortal): Establishing reactivity descriptors for platinum group metal (PGM)-free Fe-N-C catalysts for PEM fuel cells

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DOI	10.1039/d0ee01013h
	Establishing reactivity descriptors for platinum group metal (PGM)-free Fe-N-C catalysts for PEM fuel cells
	Primbs M.; Sun Y.; Roy A.; Malko D.; Mehmood A.; Sougrati M.-T.; Blanchard P.-Y.; Granozzi G.; Kosmala T.; Daniel G.; Atanassov P.; Sharman J.; Durante C.; Kucernak A.; Jones D.; Jaouen F.; Strasser P.
发表日期	2020
ISSN	17545692
起始页码	2480
结束页码	2500
卷号	13 期号:8
英文摘要	We report a comprehensive analysis of the catalytic oxygen reduction reaction (ORR) reactivity of four of today's most active benchmark platinum group metal-free (PGM-free) iron/nitrogen doped carbon electrocatalysts (Fe-N-Cs). Our analysis reaches far beyond previous such attempts in linking kinetic performance metrics, such as electrocatalytic mass-based and surface area-based catalytic activity with previously elusive kinetic metrics such as the active metal site density (SD) and the catalytic turnover frequency (TOF). Kinetic ORR activities, SD and TOF values were evaluated using in situ electrochemical NO2- reduction as well as an ex situ gaseous CO cryo chemisorption. Experimental ex situ and in situ Fe surface site densities displayed remarkable quantitative congruence. Plots of SD versus TOF ("reactivity maps") are utilized as new analytical tools to deconvolute ORR reactivities and thus enabling rational catalyst developments. A microporous catalyst showed large SD values paired with low TOF, while mesoporous catalysts displayed the opposite. Trends in Fe surface site density were linked to molecular nitrogen and Fe moieties (D1 and D2 from 57Fe Mössbauer spectroscopy), from which pore locations of catalytically active D1 and D2 sites were established. This cross-laboratory analysis, its employed experimental practices and analytical methodologies are expected to serve as a widely accepted reference for future, knowledge-based research into improved PGM-free fuel cell cathode catalysts. © 2020 The Royal Society of Chemistry.
英文关键词	Electrocatalysts; Electrolytic reduction; Iron; Iron compounds; Iron metallography; Kinetics; Knowledge based systems; Metal analysis; Oxygen reduction reaction; Platinum; Proton exchange membrane fuel cells (PEMFC); Analytical methodology; Comprehensive analysis; Laboratory analysis; Mesoporous catalysts; Platinum group metals; Reactivity descriptors; Ssbauer spectroscopies; Surface site density; Catalyst activity; catalyst; electrode; fuel cell; molecular analysis; nitrogen; platinum group element; quantitative analysis; reduction
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/189599
作者单位	Department of Chemistry, Chemical Engineering Division, Technical University of Berlin, Berlin, 10623, Germany; ICGM, Univ., Montpellier, ENSCM, Montpellier, France; Department of Chemistry, Imperial College London South Kensington, London, SW7 2AZ, United Kingdom; Department of Chemical Sciences, University of Padova, Via Marzolo 1, Padova, 35131, Italy; Department of Chemical, Biomolecular Engineering and National Fuel Cell Research Center, University of California, Irvine, CA 92697, United States; Johnson Matthey Technology Center, Blount's Court Sonning Common, Reading, RG4 9NH, United Kingdom
推荐引用方式 GB/T 7714	Primbs M.,Sun Y.,Roy A.,et al. Establishing reactivity descriptors for platinum group metal (PGM)-free Fe-N-C catalysts for PEM fuel cells[J],2020,13(8).
APA	Primbs M..,Sun Y..,Roy A..,Malko D..,Mehmood A..,...&Strasser P..(2020).Establishing reactivity descriptors for platinum group metal (PGM)-free Fe-N-C catalysts for PEM fuel cells.Energy & Environmental Science,13(8).
MLA	Primbs M.,et al."Establishing reactivity descriptors for platinum group metal (PGM)-free Fe-N-C catalysts for PEM fuel cells".Energy & Environmental Science 13.8(2020).