物理化学学报 >> 2021, Vol. 37 >> Issue (7): 2009107.doi: 10.3866/PKU.WHXB202009107

所属专题: 电催化

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CeO2/RP-PSCFM@CoFe阳极材料用于质子导体乙烷燃料电池共生乙烯和电能

樊赟1, 陈国诞1, 奚修安1, 李俊1, 王琦2, 骆静利1, 符显珠1,*()   

  1. 1 深圳大学材料学院,广东 深圳 518060
    2 中国地质大学材料科学与技术学院,北京 100083
  • 收稿日期:2020-09-30 录用日期:2020-10-30 发布日期:2020-11-05
  • 通讯作者: 符显珠 E-mail:xz.fu@szu.edu.cn
  • 作者简介:第一联系人:

    These authors contributed equally to this work and should be considered co-first authors.

  • 基金资助:
    国家自然科学基金项目(21975163)

Co-Generation of Ethylene and Electricity from Ethane by CeO2/RP-PSCFM@CoFe Anode Materials in Proton Conductive Fuel Cells

Yun Fan1, Guodan Chen1, Xiuan Xi1, Jun Li1, Qi Wang2, Jingli Luo1, Xianzhu Fu1,*()   

  1. 1 College of Material Science and Engineering, Shenzhen University, Shenzhen 518060, Guangdong Province, China
    2 School of Materials Science and Technology, China University of Geosciences, Beijing 100083, China
  • Received:2020-09-30 Accepted:2020-10-30 Published:2020-11-05
  • Contact: Xianzhu Fu E-mail:xz.fu@szu.edu.cn
  • About author:Xianzhu Fu, Email: xz.fu@szu.edu.cn; Tel.: +86-755-86392151
  • Supported by:
    the National Natural Science Foundation of China(21975163)

摘要:

固体氧化物燃料电池钙钛矿阳极材料可以通过改性获得优异的催化活性,低的极化阻抗和稳定的抗积炭能力。在此,以立方相钙钛矿Pr0.4Sr0.6Co0.2Fe0.7Mo0.1O3−δ作为阳极前驱体,然后将CeO2成功地浸渍到阳极的多孔结构中。通过原位还原技术获得了纳米合金粒子负载钙钛矿基底的复合阳极用于质子导体乙烷固体氧化物燃料电池。在氢气和乙烷气氛中,750 ℃时,燃料电池峰值功率密度分别达到253和183 mW∙cm−2。而且,在十小时的测试中燃料电池性能没有衰减反而电流密度随着时间的延长而增加,表明CeO2浸渍表现出优异的催化活性和抗积炭稳定性。同时,通过产物分析,乙烯的产率从650 ℃下的23.52%增加到750 ℃下的34.09%,并且乙烯选择性超过94%。因此改性的阳极通过析出的纳米颗粒与CeO2的协同作用,促进了燃料电池电极的催化活性和稳定性,将其运用到质子导体固体氧化物乙烷燃料电池中成功实现了乙烯与电能的共生。

关键词: 复合阳极, 浸渍, 乙烷, 共生燃料电池, 抗积炭

Abstract:

The continuous consumption and excessive use of fossil fuels promote the exploration of new energy conversion technologies. Meanwhile, the increase in the supply of ethane encourages the development of industrial technology for the production of ethylene chemical raw materials. Compared with traditional fossil fuel energy conversion equipment, solid oxide ethane cogeneration fuel cells are an efficient energy processing device. Through selective oxidation of fuel gas on the anode, the endothermic process of ethane dehydrogenation is converted into an exothermic oxidation reaction, which has a greater driving force for reaction thermodynamics, and simultaneously produces clean electricity and value-added chemicals without CO2 emissions. The anode material used for the proton conductor ethane fuel cells needs to operate stably and efficiently under hydrocarbon fuel. Consequently, excellent catalytic activity, low polarization resistance, and anti-coking stability are essential. In this work, CeO2 was uniformly impregnated into the surface of the porous cubic perovskite Pr0.4Sr0.6Co0.2Fe0.7Mo0.1O3−δ anode by wet impregnation, and then calcined and reduced to obtain a CeO2/RP-PSCFM@CoFe composite anode embedded with nanoparticles, which was successfully used in electrolyte-supported proton conductor fuel cells. CeO2 has a high ionic conductivity and transport capacity, which accelerates the transfer rate of protons on the anode and improves the catalytic reaction and transport process. Moreover, uniformly dispersed CeO2 can effectively increase the three-phase interface of the anode reaction and increase the range of reaction activity. The peak power densities before and after wet impregnation reached 172 and 253 mW·cm−2, respectively, at 750 ℃. When switching to ethane as the fuel, the peak power densities reached 136 and 183 mW·cm−2, respectively. The polarization resistance of the impregnated single cell was significantly reduced, and the catalytic activity improved. Moreover, there was no attenuation for 10 h in the long-term test. Inversely, the current density increased with the continuous reduction of the composite anode. Product analysis revealed that the yield of ethylene increased from 23.52% at 650 ℃ to 34.09% at 750 ℃, and the ethylene selectivity exceeded 94%. These results clearly show that the impregnated anode exhibited excellent catalytic activity and anti-coking ability in hydrocarbon fuels at high temperatures. Combining CoFe nanoparticles with CeO2 enhanced the electronic conductance and ionic conductance of the electrode, improved the transmission of electric energy and the efficient conversion of chemicals, thus successfully producing the cogeneration of electric energy and ethylene.

Key words: Composite anode, Impregnation, Ethane, Cogeneration fuel cells, Anti-coking

MSC2000: 

  • O646