Article(id=1320107548611555337, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320107530261479891, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20250434, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1748966400000, receivedDateStr=2025-06-04, revisedDate=1750953600000, revisedDateStr=2025-06-27, acceptedDate=null, acceptedDateStr=null, onlineDate=1792667766001, onlineDateStr=2026-10-22, pubDate=1782144000000, pubDateStr=2026-06-23, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792667766001, onlineIssueDateStr=2026-10-22, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792667766000, creator=13701087609, updateTime=1792667766000, updator=13701087609, issue=Issue{id=1320107530261479891, tenantId=1146029695717560320, journalId=1263187385517883426, year='2026', volume='54', issue='7', pageStart='2171', pageEnd='2576', issueExtLink='null', onlineDate='null', pubDate='1784476800000', pubDateStr='2026-07-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792667761625, creator='13701087609', updateTime=1792720444956, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1320328500238725499, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320107530261479891, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1320328500238725500, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320107530261479891, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=2397, endPage=2407, ext={EN=ArticleExt(id=1320107548825464842, articleId=1320107548611555337, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Performance of Triple-Conducting Na
0.15X
2.85Co
4O
9-δ Oxygen Electrode, columnId=1263922769897599102, journalTitle=Journal of the Chinese Ceramic Society, columnName=Research Articles, runingTitle=null, highlight=null, articleAbstract=
Introduction Proton-conducting solid oxide fuel cells (H-SOFCs) require highly active oxygen electrodes to enhance their electrochemical performance and stability at intermediate and low temperatures. However, conventional oxygen electrode materials often suffer from high thermal expansion coefficients and insufficient catalytic activity at reduced temperatures, making them unsuitable for H-SOFC applications. Misfit-layered oxides (MLOs) can offer a promising solution due to their unique structural and catalytic properties. In this study, a series of Na0.15X2.85Co4O9-δ (X=Ca, Sr, Ba; abbreviated as NCC, NSC, and NBC) materials were synthesized by a glycine-nitrate combustion method. These materials possess a misfit-layered structure ([X2CoO3-δ] and [CoO2-δ] layers), which reduces their thermal expansion coefficients and enhances the catalytic activity of oxygen electrodes at intermediate and low temperatures. Among the Na0.15X2.85Co4O9-δ materials, NSC exhibits the optimum performance (i.e., an electrical conductivity of 57.1 S·cm-1 at 700 ℃ in 5% (in volume fraction) H2O atmosphere, and an area-specific resistance (ASR) of 0.19 Ω·cm2 at 650 ℃ in an NSC|BZCYYb (BaZr0.1Ce0.7Y0.1Yb0.1O3-δ)|NSC symmetric cell, with only a ~2% increase in ASR after 100 h at 600 ℃). In a full-cell test with NSC|BZCYYb|Ni-BZCYYb, the oxygen electrode achieves power densities of 1273 mW·cm-2 and 362 mW·cm-2 at 650 ℃ and 500 ℃, respectively, and demonstrates a stable operation for 165 h at a constant current density of 0.54 A·cm-2 at 600 ℃. This work demonstrates that the misfit-layered Na0.15Sr2.85Co4O9-δ material has a significant promising application in H-SOFCs.
Methods In this study, three materials of the misfit-layered Na0.15X2.85Co4O9-δ (NXC, X=Ca, Sr, Ba; abbreviated as NCC, NSC, NBC) system were synthesized by a glycine-nitrate combustion method. These materials featured an alternating stacking structure composed of [X2CoO3-δ] and [CoO2-δ] layers. The NXC series electrode materials were obtained via calcination in a muffle furnace at 800 ℃ for 2 h, followed by grinding. The intrinsic properties of the materials (i.e., electrical conductivity and thermal expansion coefficient) were characterized. Electrode slurries were prepared via grinding the materials, which were then screen-printed onto BaZr0.1Ce0.7Y0.1Yb0.1O3-δ (BZCYYb) electrolyte pellets to fabricate NXC|BZCYYb|NXC symmetric cells. These symmetric cells underwent temperature sensitivity, humidity sensitivity, and stability tests. The material with the optimal comprehensive performance was selected to construct NXC|BZCYYb|Ni-BZCYYb full cells. The full cells were characterized by current density-voltage measurement, electrochemical impedance spectroscopy (EIS) at 650-500 ℃, and relaxation time (DRT) analysis.
Results and discussion Among the three materials, NCC and NSC both exhibit well-formed phases, whereas NBC produces a significant amount of the secondary phase BaCoO3-δ. The thermal expansion coefficients (TECs) of NCC and NSC are relatively low, while that of NBC is notably higher due to the high TEC of the secondary phase. In terms of electrical conductivity, NSC demonstrates the optimum performance among the three materials, achieving 40.8 S·cm-1 at 500 ℃ in dry air, which is significantly superior to those of NCC and NBC. At 650 ℃, the polarization resistances (Rp) of NCC and NSC both are 0.190 Ω·cm2, while NBC exhibits a higher Rp of 0.252 Ω·cm2, indicating that Ca- and Sr-doped electrodes possess comparable charge transfer capabilities at elevated temperatures, whereas the Ba-doped material performs slightly worse. Also, NSC displays a superior performance in both humidity sensitivity and stability tests. Based on the analysis above, NSC in the NXC series with the maximum conductivity, catalytic activity, and stability is selected as an oxygen electrode for the NSC|BZCYYb|Ni-BZCYYb full cell for subsequent testing. NSC exhibits excellent performance and stability, delivering power densities of 1273, 1095, 704, 362, 170 mW·cm-2 and 91 mW·cm-2 at 650-400 ℃. Moreover, it demonstrates a stable operation for 165 h at an applied current density of 0.54 A·cm-2, confirming its potential as an oxygen electrode for H-SOFCs.
Conclusions This study synthesized a series of misfit-layered Na0.15X2.85Co4O9-δ (NXC, X=Ca, Sr, Ba; abbreviated as NCC, NSC, and NBC) oxygen electrode materials by a glycine-nitrate combustion method. The influences of elements Ca, Sr, and Ba on the crystal structure and electrochemical properties were systematically investigated. Among the synthesized materials, Na0.15Sr2.85Co4O9-δ (NSC) demonstrated optimal electrochemical performance and stability. It exhibited an electrical conductivity of 57.1 S·cm-1 at 700 ℃ in a 5% H2O+95% air atmosphere. The NSC symmetric cell showed the lowest area-specific polarization resistances (ASR) of 0.190, 0.323, 0.590 Ω·cm2, and 0.911 Ω·cm2 at 650-500 ℃, along with excellent long-term stability. These superior characteristics were further confirmed in NSC|BZCYYb|Ni-BZCYYb full-cell tests, achieving high power densities of 1273, 1095, 704, 362 mW·cm-2 at 650-500 ℃, respectively. Moreover, the cell maintained stable operation for 165 h at an applied current density of 0.54 A·cm-2, demonstrating a remarkable stability. These results indicated that the triple-conducting (H+/O2-/e-) misfit-layered NSC material could be a highly promising oxygen electrode candidate for intermediate-to-low temperature solid oxide cells.
, authors=ZiXian WANG, Weitao JIN, Ruiqing SONG, Jiansong YUAN, Hengxi PANG, Juan ZHOU, authorsList=ZiXian WANG, Weitao JIN, Ruiqing SONG, Jiansong YUAN, Hengxi PANG, Juan ZHOU, authorCompany=null, correspAuthors=Juan ZHOU, authorNote=
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0.15X
2.85Co
4O
9-δ氧电极的制备与性能, columnId=1263922770220560512, journalTitle=硅酸盐学报, columnName=研究论文, runingTitle=null, highlight=null, articleAbstract=
质子导体固体氧化物燃料电池（H-SOFC）在中低温下氧电极的催化活性是提升H-SOFC电化学性能和稳定性的关键。但传统氧电极材料热膨胀系数较高，低温下催化活性较低，难以满足H-SOFC氧电极要求。而错配型层状结构氧化物有望提供新的解决方案。本工作通过甘氨酸燃烧法成功制备了Na0.15X2.85Co4O9-δ（X=Ca、Sr、Ba；简称NCC、NSC和NBC）系列材料，其拥有错配层状（[X2CoO3-δ]层与[CoO2-δ]层）结构，热膨胀系数较小，中低温下氧电极的催化活性较高。在Na0.15X2.85Co4O9-δ材料中，NSC展现出了最佳的性能：在5%（体积分数）H2O+95%空气气氛、700 ℃下电导率为57.1 S·cm-1，650 ℃下NSC|BZCYYb （BaZr0.1Ce0.7Y0.1Yb0.1O3-δ）|NSC对称电池极化阻抗为0.19 Ω·cm2，600 ℃下100 h后增长约2%。NSC|BZCYYb|Ni-BZCYYb全电池测试中，氧电极在650 ℃和500 ℃下功率密度分别为1273 mW·cm-2和362 mW·cm-2，并在600 ℃、0.54 A·cm-2外加电流密度下165 h保持稳定。该工作表明Na0.15Sr2.85Co4O9-δ错配层状材料在H-SOFC中的具有一定的优势。
, authors=王自贤, 金炜涛, 宋瑞卿, 袁建松, 庞恒熙, 周娟, authorsList=王自贤, 金炜涛, 宋瑞卿, 袁建松, 庞恒熙, 周娟, authorCompany=null, correspAuthors=周娟, authorNote=
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周娟（1985—），女，副教授。
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王自贤（2000—），男，硕士研究生。
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