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Preparation of Nitrogen-Doped Carbon catalyst to Oxygen Reduction Reaction and Influence of Protective Gas Flowing on Its Activity

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Chinese Journal of Chemical Physics 2016年第2期29卷 255-259,I0002页

作者：熊中平司玉军余鸿李敏娇陈茂学四川理工学院化学与制药工程学院绿色催化四川省高等学校重点实验室自贡643000

A non-precious metal catalyst MnHMTA/C to oxygen reduction reaction was prepared by py- rolyzing a precursor from manganese chloride, hexamethylenetetramine and acetylene black in nitrogen gas atmosphere. The effect of heat treatment temperature and flowing of nitrogen gas were investigated. A catalyst with the highest activity can be obtained at 700 ℃. Mn（Ⅱ） ion was changed to MnO in heat treatment, which improved the catalytic activity of the catalyst. Hexamethylenetetramine takes part in the formation of active site of the catalyst as its decomposed gases. The flowing of protective gas takes the decomposed gases out of the tube furnace and brings negative effect on the catalytic activity of the MnHMTA/C catalyst.

关键词： Oxygen reduction reaction non-precious metal catalyst Manganese Protective gas flowing

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Catalysis stability enhancement of Fe/Co dual-atom site via phosphorus coordination for proton exchange membrane fuel cell

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Nano Research 2022年第4期15卷 3082-3089页

作者： Yinuo Wang Xin Wan Jieyuan Liu Wenwen Li Yongcheng Li Xu Guo Xiaofang Liu Jiaxiang Shang Jianglan Shui School of Materials Science and Engineering Beihang UniversityBeijing 100081China Qinghai Provincial Key Laboratory of New Light Alloys Qinghai Provincial Engineering Research Center of High-Performance Light Metal Alloys and FormingQinghai UniversityXining 810016China

non-precious metal catalysts(NPMCs)are promising low-cost alternatives of Pt/C for oxygen reduction reaction(ORR),which however suffer from serious stability challenge in the devices of proton-exchange-membrane fuel cells(PEMFC).Different from the traditional strategies of increasing the degree of graphitization of carbon substrates and using less Fenton-reactive metals,we prove here that proper regulation of coordination anions is also an effective way to improve the stability of NPMC.N/P cocoordinated Fe-Co dual-atomic-sites are constructed on ZIF-8 derived carbon support using a molecular precursor of C_(34)H_(28)Cl_(2)CoFeP_(2)and a“precursor-preselected”method.A composition of FeCoN_(5)P1 is infered for the dual-atom active site by microscopy and spectroscopy *** comparing with N-coordinated references,we investigate the effect of P-coodination on the ORR catalysis of Fe-Co dual-atom catalysts in *** metals in FeCoN_(5)P1 have the lower formation energy than those in the solo N-coordinated active sites of FeCoN6 and FeN_(4),and exhibits a much better fuel cell *** anion approach provides a new way to improve the stability of dual-atom catalysts.

关键词： fuel cell oxygen reduction reaction non-precious metal catalyst dual atomic site P/N coordination

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Reduced formation of peroxide and radical species stabilises iron-based hybrid catalysts in polymer electrolyte membrane fuel cells

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Journal of Energy Chemistry 2022年第2期31卷 433-438页

作者： Dongyoon Shin Sabita Bhandari Marc FTesch Shannon ABonke Frédéric Jaouen Sonia Chabbra Christoph Pratsch Alexander Schnegg Anna K.Mechler Max Planck Institute for Chemical Energy Conversion Stiftstr.34–3645470 Mülheim an der RuhrGermany ICGM Univ.MontpellierCNRSENSCMMontpellierFrance Fritz Haber Institute of the Max Planck Society Department of Inorganic ChemistryFaradayweg 4-614195 BerlinGermany

The incorporation of Pt into an iron-nitrogen-carbon(Fe NC)catalyst for the oxygen reduction reaction(ORR)was recently shown to enhance catalyst stability without Pt directly contributing to the ORR ***,the mechanistic origin of this stabilisation remained *** is established herein with rotating ring disc experiments that the side product,H_(2)O_(2),which is known to damage FeNC catalysts,is suppressed by the presence of *** formation of reactive oxygen species is additionally inhibited,independent of intrinsic H_(2)O_(2) formation,as determined by electron paramagnetic *** electron microscopy identifies an oxidised Fe-rich layer covering the Pt particles,thus explaining the inactivity of the latter towards the *** insights develop understanding of Fe NC degradation mechanisms during ORR catalysis,and crucially establish the required properties of a precious metal free protective catalyst to improve Fe NC stability in acidic media.

关键词： Electrochemistry Fuel cells Oxygen reduction reaction non-precious metal catalyst Hybrid catalyst Stability

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The effect of temperature on ionic liquid modified Fe-N-C catalysts for alkaline oxygen reduction reaction

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Journal of Energy Chemistry 2022年第5期31卷 324-329页

作者： Thomas Wolker Kai Brunnengräber Ioanna Martinaiou Nick Lorenz Gui-Rong Zhang Ulrike I.Kramm Bastian J.M.Etzold Department of Chemistry Ernst-Berl-Institut für Technische und Makromolekulare ChemieTechnical University of Darmstadt64287 DarmstadtGermany Department of Chemistry Catalysts and Electrocatalysts GroupTechnical University of Darmstadt64287 DarmstadtGermany Graduate School of Excellence Energy Science and Engineering Technical University of Darmstadt64287 DarmstadtGermany Department of Materials and Earth Sciences Technical University of Darmstadt64287 DarmstadtGermany School of Chemical Engineering and Technology Tiangong UniversityTianjin 300387China

Modifying solid catalysts with an ionic liquid layer is an effective approach for boosting the performance of both Pt-based and non-precious metal catalysts toward the oxygen reduction reaction. While most studies operated at room temperature it remains unclear whether the IL-associated boosting effect can be maintained at elevated temperature, which is of high relevance for practical applications in low temperature fuel cells. Herein, Fe-N-C catalysts were modified by introducing small amounts of hydrophobic ionic liquid, resulting in boosted electrocatalytic activity towards the alkaline oxygen reduction reaction at room temperature. It is demonstrated that the boosting effect can be maintained and even strengthened when increasing the electrolyte temperature up to 70℃. These findings show for the first time that the incorporation of ionic liquid is a suited method to obtain advanced noble metal-free electrocatalysts that can be applied at operating temperature condition.

关键词： Oxygen reduction reaction non-precious metal catalyst Ionic liquid Fe-N-C catalyst Temperature effect

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Large specific surface area S-doped Fe–N–C electrocatalysts derived from metal–Organic frameworks for oxygen reduction reaction

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Progress in Natural Science:Materials International 2020年第6期30卷 896-904页

作者： Xiaohui Yan Xiaolin Li Cehuang Fu Chen Lin Huanming Hu Shuiyun Shen Guanghua Wei Junliang Zhang Institute of Fuel Cells School of Mechanical Engineering Shanghai Jiao Tong University Central Research Institute Shanghai Electric Group SJTU-Paris Tech Elite Institute of Technology Shanghai Jiao Tong University MOE Key Laboratory of Power Machinery and Engineering Shanghai Jiao Tong University

It is highly desired but challenging to develop platinum group metal-free electrocatalysts for oxygen reduction reaction(ORR), which can promote the commercialization of fuel cell technology. To achieve this target, we report a one-step doping method to prepare S-doped Fe–N–C catalysts using zeolite imidazole framework(ZIF-8)and iron(III) thiocyanate(Fe(SCN)3) as precursor. Different from conventional doping approach, i.e. physical mixing, Fe(SCN)3is in-situ added during ZIF-8 formation which would encapsulate Fe(SCN)3molecules inside ZIF-8 to avoid structure destruction and create potential replacement of Zn ions by Fe ions to form uniform Fe–N4 complexes. As a result, the prepared S-doped Fe–N–C catalysts own large specific surface areas with a maximum value of 1326 m2g-1and a dual-scale porous structure that benefits mass transport. Significantly, the composition-optimized catalyst exhibits superior ORR activity in both 0.1 M HCl O4electrolyte and 0.1 M KOH electrolyte, in which the half-wave potential reaches 0.81 V and 0.92 V(vs. RHE), respectively. Remarkable stability is also attained, which loses 2 m V only after 10000 potential cycles in O2-saturated 0.1 M HCl O4and remains almost constant in O2-saturated 0.1 M KOH, surpassing commercial Pt/C catalyst in both acidic and alkaline medium.

关键词： Fuel cells Oxygen reduction reaction non-precious metal catalyst Co-doping Acidic and alkaline medium

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