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Perovskite Oxyfluoride Electrode Enabling Direct Electrolyzing Carbon Dioxide with Excellent Electrochemical Performances

机译:钙钛矿氧化氧化物电极,可直接电解二氧化碳,具有优异的电化学性能

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摘要

Solid oxide electrolysis cells (SOECs) can efficiently convert the greenhouse-gas CO2 to valuable fuel CO at the cathodes. Herein, fluorine is doped into mixed ionic-electronic conducting Sr2Fe1.5Mo0.5O6-delta (SFM), to evaluate its potential use as a cathode for CO2 reduction reaction (CO2-RR). SFM retains its cubic structure after doped with fluorine, forming perovskite oxyfluoride Sr2Fe1.5Mo0.5O6-delta F0.1 (F-SFM). The substitution of oxygen by fluorine increases CO2 adsorption by a factor of approximate to 2, bulk oxygen vacancy concentration by 35-37% at 800 degrees C, and consequently enhances the surface reaction rate constant for CO2-RR and chemical bulk diffusion coefficient by factors of 2-3. The faster kinetics are also reflected by a lower polarization resistance of 0.656 omega cm(2) for F-SFM than 1.130 omega cm(2) for SFM at 800 degrees C in symmetrical cells. Furthermore, the single cell with F-SFM cathode exhibits the best CO2 electrolysis performance among the reported perovskite electrodes, achieving current density of 1.36 A cm(-2) at 1.5 V and excellent stability over 120 h at 800 degrees C under harsh conditions. The theoretical computations confirm that fluorine doping is energetically favorable to CO2 adsorption and dissociation. The present work provides a promising strategy for the design of robust cathodes for direct CO2 electrolysis in SOECs.
机译:固体氧化物电解细胞(SOECS)可以有效地将温室气体CO2有效地转化为在阴极处的有价值的燃料CO。在此,氟掺杂到混合离子 - 电子传导SR2FE1.5MO0.5O6-DELTA(SFM)中,以评估其作为CO 2还原反应的阴极的潜在用途(CO2-RR)。 SFM在掺杂氟后保持其立方体结构,形成钙钛矿氧化氢SR2FE1.5MO0.5O6-DELTA F0.1(F-SFM)。氟取代氧气将CO 2吸附在800℃下达到2,大量氧空位浓度的差分,因此通过因素增强了CO2-RR和化学批量扩散系数的表面反应速率常数2-3。对于在800℃的对称电池中,更快的动力学也通过0.656ωcm(2)的较低偏振电阻为0.656ωcm(2)的偏振电阻为0.656ωcm(2),在800摄氏度下SFM。此外,具有F-SFM阴极的单细胞在报告的钙钛矿电极中表现出最佳的CO 2电解性能,在苛刻的条件下在1.5V下实现1.5V的电流密度为1.5V,在800℃下以超过120h的稳定性。理论计算确认氟掺杂能量有利地有利于CO 2吸附和解离。本工作提供了有希望的策略,用于设计SOEC中的直接CO2电解的强大阴极。

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  • 来源
    《Advanced energy materials》 |2019年第3期|1803156.1-1803156.10|共10页
  • 作者单位

    Univ Sci & Technol China Dept Mat Sci & Engn CAS Key Lab Mat Energy Convers Hefei 230026 Anhui Peoples R China;

    Univ Bremen Inst Appl & Phys Chem D-28359 Bremen Germany;

    Univ Sci & Technol China Dept Mat Sci & Engn CAS Key Lab Mat Energy Convers Hefei 230026 Anhui Peoples R China;

    Univ Sci & Technol China Dept Mat Sci & Engn CAS Key Lab Mat Energy Convers Hefei 230026 Anhui Peoples R China;

    Univ Sci & Technol China Natl Synchrotron Radiat Lab Hefei 230029 Anhui Peoples R China;

    Univ Sci & Technol China Natl Synchrotron Radiat Lab Hefei 230029 Anhui Peoples R China;

    Univ Sci & Technol China Natl Synchrotron Radiat Lab Hefei 230029 Anhui Peoples R China;

    Univ Sci & Technol China Dept Mat Sci & Engn CAS Key Lab Mat Energy Convers Hefei 230026 Anhui Peoples R China|Anhui Estone Mat Technol Co Ltd Energy Mat Ctr Bengbu 233400 Anhui Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    anion doping; ceramic fuel electrodes; direct CO2 electrolysis; perovskite oxyfluoride; solid oxide electrolysis cells;

    机译:阴离子掺杂;陶瓷燃料电极;直接CO2电解;钙钛矿氧化物;固体氧化物电解细胞;

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