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Wormholelike mesoporous carbon supported Pt Ru catalysts toward methanol electrooxidation

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Journal of Energy Chemistry 2017年第1期26卷 200-206页

作者： Weifeng Liu Xiaoping Qin Xiongfu Zhang Zhigang Shao baolian yi State Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian Institute of Chemical Physics Chinese Academy of Sciences

Wormholelike mesoporous carbons (WMCs) with three different pore diameters (D-P), namely WMC-F7 (D-p = 8.5 nm), WMC-F30 (D-p =4.4 nm), and WMC-F0 (D-p =3.1 nm) are prepared via a modified sol-gel process. Then PtRu nanoparticles with the particle size (40 of 3.2 nm supported on WMCs are synthesized with a modified pulse microwave-assisted polyol method. It is found that the pore diameter of WMCs plays an important role in the electrochemical activity of PtRu toward alcohol electrooxidation reaction. PtRu/WMC-F7 with D-p > 2d(pt) exhibits the largest electrochemical surface area (ESA) and the highest activity toward methanol electrooxidation. With the decrease in Dp, PtRu/WMC-F30 and PtRu/WMC-F0 have much lower ESA and electrochemical activity, especially for the isopropanol electrooxidation with a larger molecular size. When D-p is more than twice d(pt), the mass transfer of reactants and electrolyte are easier, and thus more PtRu nanoparticles can be utilized and the catalysts activity can be enhanced. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

关键词： Wormholelike mesoporous carbon PtRu catalyst Pore diameter Methanol electrooxidation

Enhanced electrocatalytic performance of ultrathin PtNi alloy nanowires for oxygen reduction reaction

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Frontiers in Energy 2017年第3期11卷 260-267页

作者： Hongjie ZHANG Yachao ZENG Longsheng CAO Limeng YANG Dahui FANG baolian yi Zhigang SHAO Fuel Cell System and Engineering Laboratory Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China University of the Chinese Academy of Sciences Beijing 100039 China

In this paper, ultrathin Pt nanowires （Pt NWs） and PtNi alloy nanowires （PtNi NWs） supported on carbon were synthesized as electrocatalysts for oxygen reduction reaction （ORR）. Pt and PtNi NWs catalysts composed of interconnected nanoparticles were prepared by using a soft template method with CTAB as the surface active agent. The physical characterization and electrocatalytic perfor- mance of Pt NWs and PtNi NWs catalysts for ORR were investigated and the results were compared with the commercial Pt/C catalyst. The atomic ratio of Pt and Ni in PtNi alloy was approximately 3 to 1. The results show that after alloying with Ni, the binding energy of Pt shifts to higher values, indicating the change of its electronic structure, and that Pt3Ni NWs catalyst has a significantly higher electrocatalytic activity and good stability for ORR as compared to Pt NWs and even Pt/C catalyst. The enhanced electrocatalytic activity of Pt3Ni NWs catalyst is mainly resulted from the downshifted-band center of Pt caused by the interaction between Pt and Ni in the alloy, which facilitates the desorption of oxygen containing species （Oads or OHads） and the release of active sites.

关键词： PtNi alloy nanowires oxygen reduction reaction enhanced activity good stability

Sulfur/carbon composites prepared with ordered porous carbon for Li-S battery cathode

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Journal of Energy Chemistry 2014年第3期23卷 391-396页

作者： Xin Zhuang yingjia Liu Jian Chen Hao Chen baolian yi Lab of Advanced Rechargeable Batteries Dalian Institute of Chemical PhysicsChinese Academy of Science

Ordered porous cabon with a 2-D hexagonal structure,high specific surface area and large pore volume was synthesized through a twostep heating method using tri-block copolymer as template and phenolic resin as carbon precursor.The results indicated the electrochemical performance of the sulfur/carbon composites prepared with the ordered porous carbon was significantly affected by the pore structure of the carbon.Both the specific capacity and cycling stability of the sulfur/carbon composites were improved using the bimodal micro/meso-porous carbon frameworks with high surface area.Its initial discharge capacity can be as high as 1200 mAh·g-1 at a current density of 167.5 mA·g-1The improved capacity retention was obtained during the cell cycling as well.

关键词： lithium-sulfur battery sulfur/carbon composite ordered porous carbon bimodal micro/meso-porous carbon tri-block copolymer

Preparation and characterization of Ti_(0.7)Sn_(0.3)O_2 as catalyst support for oxygen reduction reaction

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Journal of Energy Chemistry 2014年第3期23卷 331-337页

作者： Yuan Gao Ming Hou Zhigang Shao Changkun Zhang Xiaoping Qin baolian yi Fuel Cell System and Engineering Laboratory Dalian Institute of Chemical PhysicsChinese Academy of Sciences Graduate School of Chinese Academy of Sciences

Sn-doped TiO2 nanoparticles with high surface area of 125.7 m2·g-1 are synthesized via a simple one-step hydrothermai method and explored as the cathode catalyst support for proton exchange membrane fuel cells.The synthesized support materials are studied by X-ray diffraction analysis,energy dispersive X-ray spectroscopy and transmission electron microscopy.It is found that the conductivity has been greatly improved by the addition of 30 mol%Sn and Pt nanoparticles are well dispersed on Ti0.7Sn0.3O2 support with an average size of 2.44 run.Electrochemical studies show that the Ti0.7Sn0.3O2 nanoparticles have excellent electrochemical stability under a high potential compared to Vulcan XC-72.The as-synthesized Pt/Ti0.7Sn0.3O2 exhibits high and stable electrocatalytic activity for the oxygen reduction reaction.The Pt/Ti0.7Sn0.3O2 catalyst reserves most of its electrochemically active surface area（ECA）,and its half wave potential difference is 11 mV,which is lower than that of Pt/XC-72（36 mV） under 10 h potential hold at 1.4 V vs.NHE.In addition,the ECA degradation of Pt/Ti0.7Sn0.3O2is 1.9 times lower than commercial Pt/XC-72 under 500 potential cycles between 0.6 V and 1.2 V vs.NHE.Therefore,the as synthesized Pt/Ti0.7Sn0.3O2 can be considered as a promising alternative cathode,catalyst for proton exchange membrane fuel cells.

关键词： tin titanium oxide support durability proton exchange membrane fuel cells

Development of proton-conducting membrane based on incorporating a proton conductor 1,2,4-triazolium methanesulfonate into the Nafion membrane

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Journal of Energy Chemistry 2015年第2期24卷 199-206页

作者： Jinkai Hao Xiaojin Li Shuchun Yu Yongyi Jiang Jiangshui Luo Zhigang Shao baolian yi Fuel Cell System and Engineering Laboratory Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Department of Materials Engineering Centre for Surface Chemistry and Catalysis

In this paper, 1,2,4-triazolium methanesulfonate （C_2H_4N_3^＋-CH_3SO_3^-, [Tri][MS]）, an ionic conductor, was successfully synthesized. It exhibited high ionic conductivity of 18.60 mS·cm^-1 at 140 ℃ and reached up to 36.51 mS·cm^-1 at 190 ℃. [Tri][MS] was first applied to modify Nation membrane to fabricate [Tri][MS]/Nafion membrane by impregnation method at 150 ℃. The prepared composite membrane showed high thermal stability with decomposed temperature above 200 ℃ in air atmosphere. In addition, the membrane indicated good ionic conductivity with 3.67 mS·cm^-1 at 140 ℃ and reached up to 13.23 mS·cm^-1 at 180 ℃. The structure of the [Tri][MS] and the composite membrane were characterized by FTIR and the compatibility of [Tri][MS] and Pt/C catalyst was studied by a cyclic voltammetry （CV） method. Besides, the [Tri][MS]/Nafion membrane （thickness of 65 μm） was evaluated with single fuel cell at high temperature and without humidification. The highest power density of [Tri][MS]/Nafion membrane was 3.20 mW·cm^-2 at 140 ℃ and 4.90 mW·cm^-2 at 150 ℃, which was much higher than that of Nation membrane.

关键词： high temperature PEMFC membranes triazole Nafion ionic conductor

Pt/WO_3/C nanocomposite with parallel WO_3 nanorods as cathode catalyst for proton exchange membrane fuel cells

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Journal of Energy Chemistry 2015年第1期24卷 39-44页

作者： Meiling Dou Ming Hou Zhilin Li Feng Wang Dong Liang Zhigang Shao baolian yi State Key Laboratory of Chemical Resource Engineering Beijing Key Laboratory of Electrochemical Process and Technology for MaterialsBeijing University of Chemical Technology Fuel Cell System and Engineering Laboratory Dalian Institute of Chemical Physics Chinese Academy of Sciences

Pt/WO3/C nanocomposites with parallel WO3 nanorods were synthesized and applied as the cathode catalyst for proton exchange membrane fuel cells （PEMFCs）. Electrochemical results and single cell tests show that an enhanced activity for the oxygen reduction reaction （ORR） is obtained for the Pt/WO3/C catalyst compared with Pt/C. The higher catalytic activity might be ascribed to the improved Pt dispersion with smaller particle sizes. The Pt/WO3/C catalyst also exhibits a good electrochemical stability under potential cycling. Thus, the Pt/WO3/C catalyst can be used as a potential PEMFC cathode catalyst.

关键词： tungsten oxides Pt nanoparticles catalyst proton exchange membrane fuel cells

Effect of electrode Pt-loading and cathode flow-field plate type on the degradation of PEMFC

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Journal of Energy Chemistry 2019年第8期28卷 95-103,I0005页

作者： Lijuan Qu Zhiqiang Wang Xiaoqian Guo Wei Song Feng Xie Liang He Zhigang Shao baolian yi Fuel Cell System and Engineering Group Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023 Liaoning China University of Chinese Academy of Sciences Beijing 100049 China

The electrode Pt-loading has an effect on the number of active sites and the thickness of catalyst layer,which has huge influence on the mass transfer and water management during dynamic process in PEMFCs. In this study, membrane electrode assemblies with different Pt-loadings were prepared, and PEMFCs were assembled using those membrane electrode assemblies with traditional solid plate and water transport plate as cathode flow-field plates, respectively. The performance and electrochemical surface area of cells were characterized to evaluate the membrane electrode assemblies degradation after rapid currentvariation cycles. Scanning electron microscope and transmission electron microscope were used to investigate the decay of catalyst layers and Pt/C catalyst. With the increase of Pt-loading, the performance degradation of membrane electrode assemblies will be mitigated. But higher Pt-loading means thicker catalyst layer, which leads to a longer pathway of mass transfer, and it may result in carbon material corrosion in membrane electrode assemblies. The decay of Pt/C catalyst in cathode is mainly caused by the corrosion of carbon support, and the degradation of anode Pt/C catalyst is a consequence of migration and aggregation of Pt particles. And using water transport plate is beneficial to alleviating the age of cathode Pt/C catalyst.

关键词： Proton exchange membrane fuel cell Electrode platinum loading Current-variation cycle Traditional solid plate Water transport plate

Recent progresses in H2-PEMFC at DICP

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Journal of Energy Chemistry 2019年第9期28卷 129-140页

作者： Feng Xie Zhigang Shao Ming Hou Hongmei Yu Wei Song Shucheng Sun Li Zhou baolian yi Division of Fuel Cell and Battery Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023 Liaoning China University of Chinese Academy of Sciences Beijing 100039 China

Proton exchange membrane fuel cell(PEMFC) as a power supply device has attracted wide attention in China and abroad for its advantages of high energy density, energy conversion efficiency and zero pollution.With the vigorous support of China's national policy, research institutes and enterprises have carried out extensive and pragmatic work on the basic materials, key components, stacks, auxiliary systems of PEMFCs, as well as the hydrogen station construction in order to realize the wide application of hydrogen energy.PEMFC System and Engineering Research Center of DICP is one of the earliest players in the H2-PEMFCs field.Advances have been achieved in the fields of low-platinum contained catalysts,PEMs, high-efficiency MEAs, low-cost metal bipolar plates, low-temperature and impurity air environment adaptability, stacks and systems.This paper introduces recent progresses of H2-PEMFCs at DICP in key materials, components, stacks, systems and the applications.The engineering status of proton exchange membrane water electrolysis(PEMWE) and the alkaline anion exchange membrane fuel cells(AEMFCs)are also summarized.

关键词： PEMFC Catalysts MEAs Metal bipolar plates Fuel cell stacks Low temperature startup Durability Control strategy

A new insight into the stability of nanofiber electrodes used in proton exchange membrane fuel cells

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Journal of Energy Chemistry 2020年第3期29卷 126-132页

作者： Yanyan Gao Ming Hou Liang He Manman Qi Haiping Chen Shaojing Hong Yongyi Jiang Zhigang Shao baolian yi Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100039China Guangzhou Automobile Group Co.Ltd. Automotive Engineering InstituteGuangzhou 510080GuangdongChina Anhui Mingtian Hydrogen Energy Technology Co.Ltd. Lu’an 237000AnhuiChina

The nanofiber electrodes have been considered as promising candidates for commercial proton exchange membrane fuel cells due to their high catalyst utilization and enhanced mass transport efficiency.However,for the first time our research determined that the nanofiber electrodes were restricted by the poor chemical stability of the polymer carriers.To gain further insight into the durability of nanofiber electrodes,both cyclic voltammetry aging tests and Fenton’s tests were conducted.Similar to previous reports,our research demonstrated that nanofiber electrodes showed remarkable stability in the cyclic voltammetry aging process.However,Fenton’s tests indicated that nanofibers in the electrodes would decompose easily while being attacked by reactive oxygen species such as HO·or HOO·,which greatly limits their practicability and reliability.The different performances under the two tests also demonstrated that the cyclic voltammetry aging protocols,which have been applied extensively,cannot well mirror the real operating conditions of fuel cells.

关键词： PEMFC Nanofiber electrode Stability