浸渍LaNi0.6Fe0.4O3-δ纳米颗粒对Zr0.84Y0.16O2-δ- La0.8Sr0.2Cr0.5Fe0.5O3-δ透氧膜性能的影响

doi:10.15541/jim20170115

无机材料学报 ›› 2018, Vol. 33 ›› Issue (1): 14-18.DOI: 10.15541/jim20170115

所属专题：乘风破浪的新能源材料

浸渍LaNi_0.6Fe_0.4O_3-_δ纳米颗粒对Zr_0.84Y_0.16O_2-_δ- La_0.8Sr_0.2Cr_0.5Fe_0.5O_3-_δ透氧膜性能的影响

刘雪娇^1,2, 何振宇³, 吴昊¹, 骆婷¹, 孟夑¹, 陈初升³, 占忠亮¹

1. 中国科学院上海硅酸盐研究所, 上海 200050;
2. 中国科学院大学, 北京 100049;
3.中国科学技术大学材料科学与工程系, 合肥 230026

收稿日期:2017-03-15 修回日期:2017-05-11 出版日期:2018-01-23 网络出版日期:2017-12-15
作者简介:刘雪娇(1988-), 女, 博士研究生. E-mail: xuejiao8810@student. mail.sic.ac.cn
基金资助:
国家自然科学基金(51672298) National Natural Science Foundation of China (51672298)

Influence of Impregnated Nano-scale LaNi_0.6Fe_0.4O_3-_δ Particles on the Oxygen Permeation Performance of Zr_0.84Y_0.16O_2-_δ-La_0.8Sr_0.2Cr_0.5Fe_0.5O_3-_δ Composite Membranes

LIU Xue-Jiao^1,2, HE Zhen-Yu³, WU Hao¹, LUO Ting¹, MENG Xie¹, CHEN Chu-Sheng³, ZHAN Zhong-Liang¹

1. Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China;
2. University of Chinese Academy of Sciences, Beijing 100049, China;
3. Department of Materials Sciences and Engineering, University of Science & Technology of China, Hefei 230026, China;

Received:2017-03-15 Revised:2017-05-11 Published:2018-01-23 Online:2017-12-15
Supported by:
National Natural Science Foundation of China (51672298)

摘要/Abstract

摘要：

采用流延-共压-共烧结法制备了具有多孔|致密|多孔Zr_0.84Y_0.16O_2-_δ-La_0.8Sr_0.2Cr_0.5Fe_0.5O_3-_δ (YSZ-LSCF)结构的透氧膜和多孔YSZ-LSCF|致密YSZ-LSCF|致密YSZ|致密YSZ-LSCF|多孔YSZ-LSCF结构的固体氧化物燃料电池。采用浸渍法在多孔层内壁上沉积了具有高催化活性的LaNi_0.6Fe_0.4O_3-_δ (LNF)纳米颗粒, 随着LNF浸渍量的提高, 会在多孔层内壁上形成连续的导电网格, 增加电化学反应活性位点, 进而显著改善电极性能。当LNF浸渍量为12wt%时, 电极性能达到最优, 在800℃时阴极和阳极极化阻抗分别为0.26和0.08 Ω∙cm², 在空气/CH₄梯度中氧渗透速率为7.6 mL/(cm²∙min), 比未浸渍前提高了14倍。阻抗谱分析表明空气侧氧还原反应中的电荷转移反应是氧渗透过程的速率控制步骤。

关键词: 透氧膜, 甲烷部分氧化, 纳米结构, 催化剂

Abstract:

This paper reported on the fabrication of tri-layered oxygen transport membranes, “porous|dense|porous” Zr_0.84Y_0.16O_2-δ-La_0.8Sr_0.2Cr_0.5Fe_0.5O_3-δ (YSZ-LSCF), by the tape casting, tape lamination and co-firing techniques. Catalytically active nano-scale particles of LaNi_0.6Fe_0.4O_3-δ (LNF) were impregnated into the porous scaffolds. In order to quantatively determine the resistances of the oxygen reduction or evolution reactions against oxygen permeation, an additional dense YSZ layer was introduced inside the dense YSZ-LSCF permeation layer. Electrochemical measurements on the resulting five-layered solid oxide fuel cells showed a large reduction in the interfacial polarization resistances at the presence of these LNF catalysts, with the lowest values observed at the LNF loadings of 12wt%. In particular, the cathodic and anodic polarization resistances were 0.26 and 0.08 Ω·cm² at 800℃, respectively. The oxygen permeation flux under the air/CH₄ gradient was 7.6 mL/(cm²·min), which was 14 times higher than the measured value for the blank YSZ-LSCF membrane. Further impedance analysis indicated that the charge transfer step during oxygen reduction may limit the overall oxygen permeation process.

Key words: oxygen transport membranes, partial oxidation of methane, nanostructures, catalysts

中图分类号:

TQ028.8

刘雪娇, 何振宇, 吴昊, 骆婷, 孟夑, 陈初升, 占忠亮. 浸渍LaNi_0.6Fe_0.4O_3-_δ纳米颗粒对Zr_0.84Y_0.16O_2-_δ- La_0.8Sr_0.2Cr_0.5Fe_0.5O_3-_δ透氧膜性能的影响[J]. 无机材料学报, 2018, 33(1): 14-18.

LIU Xue-Jiao, HE Zhen-Yu, WU Hao, LUO Ting, MENG Xie, CHEN Chu-Sheng, ZHAN Zhong-Liang. Influence of Impregnated Nano-scale LaNi_0.6Fe_0.4O_3-_δ Particles on the Oxygen Permeation Performance of Zr_0.84Y_0.16O_2-_δ-La_0.8Sr_0.2Cr_0.5Fe_0.5O_3-_δ Composite Membranes[J]. Journal of Inorganic Materials, 2018, 33(1): 14-18.

图/表 5

图1 透氧膜(a)、燃料电池(b)及其多孔电极(c)~(f)微观结构的扫描电镜照片

Fig. 1 SEM images of (a) OTM, (b) SOFC, (c) L4, (d) L8, (e) L12, and (f) L16

图2 (a) L0和(b) L12样品在空气/空气中的阻抗谱

Fig. 2 EIS plots of (a) L0 and (b) L12 tested at air/air gradients

图3 (a) L0和(b) L12样品在空气/甲烷气氛中的阻抗谱

Fig. 3 EIS plots of (a) L0 and (b) L12 tested at air/CH4 gradients

图4 (a) L0和(b) L12样品在空气/甲烷气氛中的伏安曲线

Fig. 4 Voltage-current curves of (a) L0 and (b) L12 tested at air/CH4 gradients

图5 不同LNF含量时透氧膜的(a)阻抗数值和(b)氧渗透速率与开路电压

Fig. 5 (a) Resistances and (b) oxygen permeation flux & open circuit voltage of OTMs with varied LNF loadings

参考文献 13

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浸渍LaNi_0.6Fe_0.4O_3-_δ纳米颗粒对Zr_0.84Y_0.16O_2-_δ- La_0.8Sr_0.2Cr_0.5Fe_0.5O_3-_δ透氧膜性能的影响

Influence of Impregnated Nano-scale LaNi_0.6Fe_0.4O_3-_δ Particles on the Oxygen Permeation Performance of Zr_0.84Y_0.16O_2-_δ-La_0.8Sr_0.2Cr_0.5Fe_0.5O_3-_δ Composite Membranes

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