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Science Bulletin 2017年第23期62卷 1602-1608页

作者： Ping Song Heather M.Barkholtz Ying Wang Weilin Xu Dijia Liu Lin Zhuang State Key Laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of Sciences Chemical Sciences and Engineering Division Argonne National Laboratory College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University

We demonstrate a new and simple method for pre-treating the carbon material and iron precursor to prepare oxygen reduction reaction(ORR) catalysts, which can produce super-high performance and stability in alkaline solution, with high performance in acid solution. This strategy using cheap materials is simply controllable. Moreover, it has achieved smaller uniform nanoparticles to exhibit high stability, and the synergetic effect of Fe and N offered much higher performance in ORR than commercial Pt/C, with high maximum power density in alkaline and acid fuel cell test. So it can make this kind of catalysts be the most promising alternatives of Pt-based catalysts with best performance/price.

关键词： Pre-treatment Uniform nanoparticle Super-high performance High stability Fuel cell

Fe,Cu-codoped metal-nitrogen-carbon catalysts with high selectivity and stability for the oxygen reduction reaction

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Chinese Chemical Letters 2021年第1期32卷 506-510页

作者： Yuemin Wang Ergui Luo Xian Wang Qinglei Meng Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China University of Science and Technology of China Hefei 230026China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Metal-nitrogen-carbon materials(M-N-C) are non-noble-metal-based alternatives to platinum-based catalysts and have attracted tremendous attention due to their low-cost,high abundance,and efficient catalytic performance towards the oxygen reduction reaction(ORR).Among them,Fe-based materials show remarkable ORR activity,but they are limited by low selectivity and low *** address these issues,herein,we have synthesized FeCu-based M-N-C catalysts,inspired by the bimetal center of cytochrome c oxidase(CcO).In acidic media,the selectivity was notably improved compared with Febased materials,with peroxide yields less than 1.2%(<1/3 of the hydrogen peroxide yields of Fe-N-C catalysts).In addition to Cu-N-C catalysts which can catalytically reduce hydrogen peroxide,the reduction current of hydrogen peroxide using FeCu-N-C-20 exceeded that of Fe-N-C by about 6% when the potential was greater than 0.4 ***,FeCu-based M-N-C catalysts suffered from only a15 mV attenuation in their half-wave potentials after 10,000 cycles of accelerated degradation tests(ADT),while there was a 30 mV negative shift for ***,we propose that the H_(2)O_(2) released from Fe-Nx sites or N-doped carbon sites would be reduced by adjacent Cu-Nx sites,re sulting in low H_(2)O_(2) yields and high stability.

关键词： Fuel cell Oxygen reduction reaction Fe Cu-codoped metal-nitrogen-carbon catalysts High selectivity High stability

Tuning the electronic structure of platinum nanocrystals towards high efficient ethanol oxidation

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Chinese Journal of Catalysis 2019年第12期40卷 1904-1911页

作者： Sheng Zhang Hai Liu Na Zhang Rong Xia Siyu Kuang Geping Yin Xinbin Ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Centre of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China State Key Laboratory of Urban Water Resource and Environment School of Chemical Engineering&TechnologyHarbin Institute of TechnologyHarbin 150001HeilongjiangChina Beijing Aerospace Propulsion Institute Beijing 100076China

Direct ethanol fuel cell is a promising low temperature fuel cell,but its development is hindered by sluggish kinetics of anode catalysts for ethanol *** a high efficient platinum/tin oxide/Graphene nanocomposite is synthesized through a facile and environmentally benign *** structure and morphology are carefully characterized by X-ray diffraction and Transmission electron microscopy,showing a clear platinum/tin oxide heterostructure uniformly dispersed on graphene *** catalyst demonstrates the highest activity among the reported catalysts and much higher durability towards ethanol oxidation compared to conventional platinum *** ultrahigh activity originates from promoted removal of poisoning carbon monoxide immediate species on platinum due to a strong electronic donating effect from both tin oxide and graphene,which is fully supported by carbon monoxide stripping and X-ray photoelectron spectroscopy *** platinum/tin oxide/Graphene appears to be a promising candidate for ethanol oxidation electrocatalysts.

关键词： Platinum nanocrystals Ethanol oxidation Electrocatalyst Pt/tin oxide heterostructure Electronic effect

Recent progress on single-molecule nanocatalysis based on single-molecule fluorescence microscopy

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Science Bulletin 2017年第4期62卷 290-301页

作者： Yuwei Zhang Tao Chen Ping Song Weilin Xu State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Provincial Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SdencesChangchun 130022China Graduate University of Chinese Academy of Sciences Beijing 100049China

Understanding the heterogeneous catalytic properties of nanoparticles is of great significance for the development of high efficient nanocatalysts, but the intrinsic heterogeneities of nanocatalysts were always covered in traditional ensemble studies. This issue can be overcome if one can follow the catalysis of individual nanoparticles in real time. This paper mainly summarizes recent developments in single- molecule nanocatalysis at single particle level in Changchun Institute of Applied Chemistry, Chinese Academy of Sciences. These developments include the revealing of catalytic kinetics of different types （plane ＆ edge） of surface atoms on individual Pd nanocubes, the observing of in situ deactivation of indi- vidual carbon-supported Pt nanoparticles during the electrocatalytic hydrogen-oxidation reaction, and the measurement of catalytic activation energies on single nanocatalysts for both product formation process and dissociation process, etc. These studies further indicate the advantages or unique abilities of single-molecule methods in the studies of nanocatalvsis or even chemical reactions.

关键词： Single-molecule nanocatalysis Single-molecule fluorescence microscopy Activation energy Electrocatalysis Super-resolution imaging

Highly active PtAu alloy surface towards selective formic acid electrooxidation

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Journal of Energy Chemistry 2019年第10期28卷 157-162页

作者： Liang Liang Fateev Vladimir Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina University of Chinese Academy of Sciences Beijing 100039China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022JilinChina State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina National Research Center“Kurchatov Institute” Kurchatov sq.1MoscowRussia

The electrochemical oxidation of formic acid has been attracting significant attention in the past few years due to the great potential prospect of direct formic acid fuel cell (DFAFC) in applications, including high theoretical open circuit potential (1.48 V), low fuel crossover, high practical power densities at low temperature, facilitating of proton transport in catalyst layers and low toxicity [1-5].

关键词： Formic acid oxidation PtAu Electrocatalysis DFAFC Nanostructure

Low-temperature synthesis of nitrogen doped carbon nanotubes as promising catalyst support for methanol oxidation

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Journal of Energy Chemistry 2019年第1期28卷 118-122页

作者： Liang Liang Meiling Xiao Jianbing Zhu Junjie Ge Changpeng Liu Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences Jilin Province Key Laboratory of Low Carbon Chemical Power Sources StateState Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

The electrochemical methanol oxidation reaction(MOR) is of paramount importance for direct methanol fuel cell(DMFC) application, where efficient catalysts are required to facilitate the complicated multiple charge transfer process. The catalyst support not only determines the dispersion status of the catalysts particles, but also exerts great influence on the electronic structure of the catalysts, thereby altering its intrinsic activity. Herein, we demonstrated that nitrogen atoms, assisted by the pre-treatment of carbon matrix with oxidants, can be easily doped into carbon nanotubes at low temperature. The obtained nitrogen-doped carbon nanotubes can effectively improve the dispersion of the supported platinum nanoparticles and facilitate the MOR by modifying the electronic structure of platinum atoms,through catalyst-support interaction.

关键词： Methanol oxidation Carbon nanotubes Hydrothermal method Nitrogen doping

A review of applications of poly(diallyldimethyl ammonium chloride) in polymer membrane fuel cells: From nanoparticles to support materials

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Chinese Journal of Catalysis 2016年第7期37卷 1025-1036页

作者：杜磊孔凡鹏陈广宇杜春雨高云智尹鸽平哈尔滨工业大学化工与化学学院城市水资源与水环境国家重点实验室黑龙江哈尔滨150090 哈尔滨工业大学化工与化学学院特种电源研究所黑龙江哈尔滨150001

Polymer membrane fuel cells represent important sustainable energy devices because their operation involves zero emissions and low temperatures and their components exhibit low toxicity. Among the various components of such cells, the electrocatalyst plays the vital role of enhancing the output power density and/or working lifetime. Over the past several decades, numerous strategies have been proposed to address the challenges of electrocatalyst activity and/or durability. Herein, we review the applications of polyelectrolytes in electrocatalysts, including the enhancement of both catalytic nanoparticles and support materials. The effects of polyelectrolytes with regard to controlling the size, composition and morphology of catalytic nanoparticles, as well as the modification of support materials were summarized. In addition, the future possibilities for the research and development of polyelectrolytes in the field of catalyst design and synthesis are discussed.

关键词： PolyelectrolyteNanoparticleSupportControllable synthesisFunctionalization

Recent advances in active sites identification and regulation of M-N/C electro-catalysts towards ORR

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Science China Chemistry 2019年第6期62卷 669-683页

作者： Jie Liu Zhao Jin Xian Wang Junjie Ge Changpeng Liu Wei Xing State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences University of Science and Technology of China Laboratory of Advanced Power Sources Changchun Institute of Applied Chemistry Chinese Academy of Sciences Jilin Province Key Laboratory of Low Carbon Chemical Power Sources

Transition metal and nitrogen co-doped carbon(M–N/C) catalysts are recognized as the most prospective alternatives for platinum-based electro-catalysts towards oxygen reduction reaction(ORR) in polymer electrolyte fuel cells. Recently, significant progress has been achieved in the identification and regulation of active sites of this kind of catalysts. In this mini review,we summarize the techniques and strategies to identify active sites in M–N/C catalysts, the main debates on active sites types, the measurement method for active site density, the reactivity descriptors for M–N/C catalysts, and directions to the design of ORR M–N/C catalysts.

关键词： ORR electro-catalysts M–N/C active sites

Correlating Fe source with Fe-N-C active site construction： Guidancefor rational design of high-performance ORR catalyst

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Journal of Energy Chemistry 2018年第6期27卷 1668-1673页

作者： Liqin Gao Meiling Xiao Zhao Jin Changpeng Liu Jianbing Zhu Junjie Ge Wei Xing State Key Laboratory of Electroanalytical Chemistry Changehun Institute of Applied Chemistry Chinese Academy of Science Changchun 130022Jilin China University of Chinese Academy of Sciences Beijing 100039 China Laboratory of Advanced Power Sources Changchun Institute of Applied Chemistry Changchun 130022 Jilin China

Pyrolyzed Fe-Nx/C materials derived from Fe-doped ZIF-8 are recently emerged as promising alternativesto noble metal platinum-based catalysts towards oxygen reduction reaction （ORR） and elucidating the de-pendacne of Fe source on the active site structure and final ORR performance is highly desirbale for fur-ther development of these materials. Here, we designed and synthesized a series of Fe-N-C catalysts usingZIF-8 and various iron salts （Fe（acac）3, FeCI3, Fe（NO3）3） as precusors. We found that the iron precursors,mainly the molecular size, hydrolysis extent, do play a major role in determining the final morphology ofFe, namely forming the Fe-Nx coordination or Fe3C nanoparticles, as well as the site density, therefore,significantly affecting the ORR activity. Among the three iron sources, Fe（acac）3 is most advantageous tothe preferential formation of single-atom Fe-Nx active sites and the derived catalyst demonstrated bestORR performance.

关键词： Carbon-nitrogen-coordinated iron (FEN4) Oxygen reduction reaction Iron source Molecular size Hydrolysis

Hydrogen etching induced hierarchical meso/micro-pore structure with increased active density to boost ORR performance of Fe-N-C catalyst

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Journal of Energy Chemistry 2019年第8期28卷 17-23,I0002页

作者： Liqin Gao Meiling Xiao Zhao Jin Changpeng Liu Junjie Ge Wei Xing State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of ScienceChangchun 130022 Jilin China University of Chinese Academy of Sciences Beijing 100039 China Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChangchun 130022 Jilin China

Rational regulation on pore structure and active site density plays critical roles in enhancing the performance of Fe-N-C catalysts. As the microporous structure of the carbon substrate is generally regarded as the active site hosts, its hostility to electron/mass transfer could lead to the incomplete fulfillment of the catalytic activity. Besides, the formation of inactive metallic Fe particles during the conventional catalyst synthesis could also decrease the active site density and complicate the identification of real active site. Herein, we developed a facial hydrogen etching methodology to yield single site Fe-N-C catalysts featured with micro/mesoporous hierarchical structure. The hydrogen concentration in pyrolysis process was designated to effectively regulate the pore structure and active site density of the resulted *** optimized sample achieves excellent ORR catalytic performance with an ultralow H2O2 yield(1%)and superb stability over 10,000 cycles. Our finding provides new thoughts for the rational design of hierarchically porous carbon-based materials and highly promising non-precious metal ORR catalysts.

关键词： Hierarchical meso/micro-pore structure Hydrogen etching Single site Fe-N-C catalysts Carbon-nitrogen-coordinated iron(FeN4) Oxygen reduction reaction