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Establishing reactivity descriptors for platinum group metal (PGM)-free Fe–N–C catalysts for PEM fuel cells
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2020-06-24 , DOI: 10.1039/d0ee01013h Mathias Primbs 1, 2, 3, 4, 5 , Yanyan Sun 1, 2, 3, 4, 5 , Aaron Roy 6, 7, 7, 8, 9 , Daniel Malko 1, 10, 11, 12 , Asad Mehmood 1, 10, 11, 12 , Moulay-Tahar Sougrati 6, 7, 7, 8, 9 , Pierre-Yves Blanchard 6, 7, 7, 8, 9 , Gaetano Granozzi 13, 14, 15, 16 , Tomasz Kosmala 13, 14, 15, 16 , Giorgia Daniel 13, 14, 15, 16 , Plamen Atanassov 17, 18, 19, 20 , Jonathan Sharman 12, 21, 22, 23 , Christian Durante 13, 14, 15, 16 , Anthony Kucernak 1, 10, 11, 12 , Deborah Jones 6, 7, 7, 8, 9 , Frédéric Jaouen 6, 7, 7, 8, 9 , Peter Strasser 1, 2, 3, 4, 5
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2020-06-24 , DOI: 10.1039/d0ee01013h Mathias Primbs 1, 2, 3, 4, 5 , Yanyan Sun 1, 2, 3, 4, 5 , Aaron Roy 6, 7, 7, 8, 9 , Daniel Malko 1, 10, 11, 12 , Asad Mehmood 1, 10, 11, 12 , Moulay-Tahar Sougrati 6, 7, 7, 8, 9 , Pierre-Yves Blanchard 6, 7, 7, 8, 9 , Gaetano Granozzi 13, 14, 15, 16 , Tomasz Kosmala 13, 14, 15, 16 , Giorgia Daniel 13, 14, 15, 16 , Plamen Atanassov 17, 18, 19, 20 , Jonathan Sharman 12, 21, 22, 23 , Christian Durante 13, 14, 15, 16 , Anthony Kucernak 1, 10, 11, 12 , Deborah Jones 6, 7, 7, 8, 9 , Frédéric Jaouen 6, 7, 7, 8, 9 , Peter Strasser 1, 2, 3, 4, 5
Affiliation
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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.
中文翻译：
建立用于PEM燃料电池的不含铂族金属（PGM）的Fe–N–C催化剂的反应性描述符
我们报告了当今四种最活跃的基准铂族无金属（无PGM）铁/氮掺杂碳电催化剂（Fe–N–Cs）的催化氧还原反应（ORR）反应性的综合分析。我们的分析远远超出了以往将动力学性能指标（如基于电催化质量和表面积的催化活性）与先前难以捉摸的动力学指标（如活性金属位点密度（SD）和催化转换频率（TOF））联系起来的尝试。利用动力学ORR活动，SD和TOF值进行评价原位电化学NO 2 -还原以及一个易地气态CO低温化学吸附。实验性的非原位和原位铁表面位点密度显示出显着的定量一致性。SD与TOF的关系图（“反应性图”）被用作新的分析工具来反卷积ORR反应性，从而促进合理的催化剂开发。微孔催化剂显示出较大的SD值，而TOF较低，而中孔催化剂显示出相反的结果。铁表面位点密度的趋势与分子氮和铁部分有关（来自57的D1和D2FeMössbauer光谱），由此确定了具有催化活性的D1和D2位的孔位置。这项跨实验室的分析，其采用的实验方法和分析方法有望作为将来对改进的无PGM燃料电池阴极催化剂进行基于知识的研究的参考。
更新日期：2020-08-14
中文翻译：
建立用于PEM燃料电池的不含铂族金属（PGM）的Fe–N–C催化剂的反应性描述符
我们报告了当今四种最活跃的基准铂族无金属（无PGM）铁/氮掺杂碳电催化剂（Fe–N–Cs）的催化氧还原反应（ORR）反应性的综合分析。我们的分析远远超出了以往将动力学性能指标（如基于电催化质量和表面积的催化活性）与先前难以捉摸的动力学指标（如活性金属位点密度（SD）和催化转换频率（TOF））联系起来的尝试。利用动力学ORR活动，SD和TOF值进行评价原位电化学NO 2 -还原以及一个易地气态CO低温化学吸附。实验性的非原位和原位铁表面位点密度显示出显着的定量一致性。SD与TOF的关系图（“反应性图”）被用作新的分析工具来反卷积ORR反应性，从而促进合理的催化剂开发。微孔催化剂显示出较大的SD值，而TOF较低，而中孔催化剂显示出相反的结果。铁表面位点密度的趋势与分子氮和铁部分有关（来自57的D1和D2FeMössbauer光谱），由此确定了具有催化活性的D1和D2位的孔位置。这项跨实验室的分析，其采用的实验方法和分析方法有望作为将来对改进的无PGM燃料电池阴极催化剂进行基于知识的研究的参考。
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