Preparation and Electrochemical Performance of Pr0.8Sr0.2Fe0.7Ni0.3O3-δ ⁃Pr1.2Sr0.8Ni0.6Fe0.4O4+δ Composite Cathode

doi:10.19894/j.issn.1000-0518.210148

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (5): 797-808.DOI: 10.19894/j.issn.1000-0518.210148

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Preparation and Electrochemical Performance of Pr_0.8Sr_0.2Fe_0.7Ni_0.3O_3-_δ ⁃Pr_1.2Sr_0.8Ni_0.6Fe_0.4O₄₊_δ Composite Cathode

Yu MENG, Qing ZHANG, Wen-Hao PENG, Xiao-Fei ZHU(), De-Feng ZHOU()

School of Chemistry and Life Science，Changchun University of Technology，Changchun 130012，China

Received:2021-03-26 Accepted:2021-07-19 Published:2022-05-01 Online:2022-05-24
Contact: Xiao-Fei ZHU,De-Feng ZHOU
About author:defengzhou65@126.com
zhuxiaofei@ccut.edu.cn
Supported by:
the National Natural Science Foundation of China(21471022);Jilin Provincial Science Research Foundation of China(20190201230JC);the 13th Five?Year Plan for Science & Technology Research is sponsored by Department of Education of Jilin Province(JJKH20200647KJ)

Abstract

Abstract:

Single-phase Pr_0.8Sr_0.2Fe_0.7Ni_0.3O_3-_δ （PSFN₁₁₃） and Pr_1.2Sr_0.8Ni_0.6Fe_0.4O₄₊_δ （PSNF₂₁₄） were prepared via a sol-gel method， and the PSFN₁₁₃-PSNF₂₁₄ heterogeneous composite cathode was prepared via mixing the two components with the mass ratio of 3∶7. The effects of hetero-interface on the structure and properties of the samples were systematically studied， and the potential of PSFN₁₁₃-PSNF₂₁₄ as an IT-SOFC（intermediate temperature solid oxide fuel cell） cathode was evaluated. The results show that the two phases of the heterogeneous composite material has good chemical and thermal stability. In addition， the heterogeneous composite material has good compatibility and interfacial adhesion with the GDC（Ce_0.8Gd_0.2O_1.9） electrolyte， so it has long-term operating stability. Meanwhile， PSNF₁₁₃ is added to PSFN₂₁₄ to form a heterogeneous mixture， which can increase the oxygen vacancy content and improve the oxygen ion transmission of PSFN₁₁₃. In addition， two-phase particles are tightly entangled to maximize the formation of hetero-interfaces and increase the specific surface area. At 800 ℃， the polarization resistance of PSFN₁₁₃-PSNF₂₁₄ is 0.053 Ω·cm²， which is only 41% of PSFN₁₁₃'s resistance and 61% of PSNF₂₁₄'s resistance. The maximum power density of the corresponding single cell is 496.80 mW/cm²， which is 2.5 times of PSFN₁₁₃'s density_{and 1.6 times of PSNF₂₁₄'s density. The voltage decay rate after 60 h long-term stability test is only 0.07%/h. Therefore， the excellent performance and outstanding stability of PSFN₁₁₃-PSNF₂₁₄ heterogeneous composite cathode make it a candidate material for IT-SOFC cathode.}

Key words: Intermediate-temperature solid oxide fuel cell, Cobalt-free composite cathode, Hetero-interface, Electrochemical performance

CLC Number:

O646

Yu MENG, Qing ZHANG, Wen-Hao PENG, Xiao-Fei ZHU, De-Feng ZHOU. Preparation and Electrochemical Performance of Pr_0.8Sr_0.2Fe_0.7Ni_0.3O_3-_δ ⁃Pr_1.2Sr_0.8Ni_0.6Fe_0.4O₄₊_δ Composite Cathode[J]. Chinese Journal of Applied Chemistry, 2022, 39(5): 797-808.

Figures/Tables 11

Fig.1 （A） XRD patterns of all samples；（B） XRD patterns of PSFN113-PSNF214 at different calcination temperatures；（C） XRD patterns of PSFN113-PSNF214 and GDC；（D） XRD patterns of NiO and GDC

Fig.2 TGA curves of PSFN113 （a）， PSNF214 （b） and PSFN113-PSNF214 （c）

Fig.3 FE-SEM images of （A） PSFN113，（B） PSNF214，（C） PSFN113-PSNF214 powders and （D） N2 adsorption desorption curves of all samples

Fig.4 （A） Bright field TEM image，（B） HR-TEM image and （C） Performance improvement mechanism diagram of PSFN113-PSNF214 heterogeneous composite cathode （the yellow solid line represents the interface between PSFN113 and PSNF214）

Fig.5 X-ray spectrum analysis of all samples （A） O，（B） Pr，（C） Fe，（D） Ni

Table 1 Contents of relevant elements obtained from XPS spectrum analysis

阴极 Cathode	PSFN₁₁₃	PSNF₂₁₄	PSFN₁₁₃?PSNF₂₁₄
O_lattice	22.1%	16.6%	9.3%
O_surface	77.9%	83.4%	90.7%
Pr⁴⁺	75.2%	75.5%	70.3%
Pr³⁺	24.8%	24.5%	29.7%
Fe⁴⁺	54.7%	63.0%	62.8%
Fe³⁺	45.3%	37.0%	37.2%
Ni³⁺	15.8%	11.8%	10.3%
Ni²⁺	84.2%	88.2%	89.7%

Fig.6 Electrochemical impedance spectra of symmetrical cells：（A） 500 ℃，（B） 600 ℃，（C） 700 ℃，（D） 800 ℃；（E） The change curves of polarization resistance with temperature and （F） the corresponding Arrhenius curves

Fig.7 Cross-sectional SEM images of symmetrical cells with （A） PSFN113，（B） PSNF214 and （C） PSFN113-PSNF214 cathode after EIS test

Fig.8 I?V?P curves of single cells： I-V curves at （A） 500 ℃，（B） 600 ℃，（C） 700 ℃，（D） 800 ℃；（E） Power density change curves with temperature；（F） Long-term stability test curve of a single cell constructed with PSFN113-PSNF214 cathode

Table 2 Comparison and summary of the maximum power density of single cells with different cathode materials reported in the literature

阴极 Cathode	电池构造 Cell configuration	最大功率密度 PPD/（W·cm^-2）	温度 Temperature/℃	参考文献 Reference
*Nd_0.5Ba_0.5Fe_0.9Co_0.1O_3-_δ	Ni?BCZD/BCZD/NBFCo	390	700	30
La_0.3Sr_0.7Ti_0.3Fe_0.70O_3-_δ	LSTF/SDC/YSZ/SDC/LSTF	374	900	31
*Nd_1.7Ca_0.3NiO₄₊_δ	NiO?GDC/GDC/GDC?Nd_1.7Ca_0.3NiO₄	188	800	32
*La_1.5Pr_0.5Ni_0.8Co_0.2O₄₊_δ	LPNCO/CGD/YSZ/Ni?YSZ	385	700	33
*Pr₂Ni_0.5Mn_0.5O_4-_δ	NiO?YSZ/YSZ/GDC/PNM	485	800	29
*Bi_0.5Ba_0.5FeO_3-_δ ?Ba（Zr_0.1Ce_0.7Y_0.2）O₃	NiO?BZCY/BZCY/BBFO?BZCY	120	700	34
Ba_0.5Sr_0.5Co_0.8Fe_0.2O_3-_δ ?Ce_0.8Sm_0.2O_2-_δ	LSCF?SDC/SDC/YSZ/SDC/BSCF?SDC	290	850	35
Pr₂NiO₄?40%Sm_0.2Ce_0.8O_1.9	PNO?40SDC/SDC/PNO?40SDC	375	800	36
La_0.6Sr_0.4Co_0.2Fe_0.8O_3-_δ ?Gd_0.1Ce_0.9O_2-_δ	SNNV10?GDC/GDC/LSCF?GDC	280	650	37
La_0.4Sr_0.6Co_0.2Fe_0.7Nb_0.1O_3-_δ ?Gd_0.1Ce_0.9O_2-_δ	LSCFN?GDC/GDC/YSZ/GDC/LSCFN?GDC	348	850	38
PSFN_113-214（5∶5）	NiO?GDC/GD C/PSFN_113-214（5∶5）	496.80	800	This work

Fig.9 （A） Comparison of cathode XRD images before and after long-term stability test；（B） SEM image of heterogeneous composite cathode powder before test；（C） SEM image of heterogeneous composite cathode powder after test

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Preparation and Electrochemical Performance of Pr_0.8Sr_0.2Fe_0.7Ni_0.3O_3-_δ ⁃Pr_1.2Sr_0.8Ni_0.6Fe_0.4O₄₊_δ Composite Cathode

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