Y2O3与Al2O3负载钴催化剂的氨分解性能差异机理研究

doi:10.12422/j.issn.1006-396X.2026.04.002

石油化工高等学校学报 ›› 2026, Vol. 39 ›› Issue (4): 13-21.DOI: 10.12422/j.issn.1006-396X.2026.04.002

Y₂O₃与Al₂O₃负载钴催化剂的氨分解性能差异机理研究

曹艺茹¹(), 许慧琳¹, 李建宇¹, 金莹莹¹, 罗燕², 陈洪锋², 陈勇³, 刘雪松¹()

^1.绍兴大学化学化工学院，浙江绍兴 312000
^2.绍兴市质量技术监督检测院，浙江绍兴 312000
^3.浙江海亮环境材料有限公司，浙江诸暨 311800

收稿日期:2025-10-20 修回日期:2025-12-08 出版日期:2026-08-25 发布日期:2026-07-20
通讯作者: 刘雪松
作者简介:曹艺茹（2003-），女，硕士研究生，从事能源环境材料方面的研究；E-mail：1007003320@qq.com。
基金资助:
国家自然科学基金项目(52370115);国家级大学生创新项目(202410349068);浙江省基础公益研究计划项目(LTGS23B070002);诸暨市科技计划项目(2023J07)

Mechanism Study on the Difference in Ammonia Decomposition Performance between Co Catalysts Supported on Y₂O₃ and Al₂O₃

Yiru CAO¹(), Huilin XU¹, Jianyu LI¹, Yingying JIN¹, Yan LUO², Hongfeng CHEN², Yong CHEN³, Xuesong LIU¹()

^1.College of Chemistry and Chemical Engineering，Shaoxing University，Shaoxing Zhejiang 312000，China
^2.Shaoxing Institute of Quality & Technical Supervision and Testing，Shaoxing Zhejiang 312000，China
^3.Zhejiang Hailiang Environmental Materials Co. ，Ltd. ，Zhuji Zhejiang 311800，China

Received:2025-10-20 Revised:2025-12-08 Published:2026-08-25 Online:2026-07-20
Contact: Xuesong LIU

摘要/Abstract

摘要：

氨分解制氢是实现“碳中和社会”的重要路径，其催化效率受载体材料调控作用的显著影响。基于Al和Y元素电子结构相似但分属主族和副族的特性，系统对比了Y₂O₃和Al₂O₃载体在Co基催化剂中的差异化机制；通过XRD、BET、SEM、XPS、H₂-TPR、NH₃-TPD对催化剂进行了表征。结果表明，虽然Al和Y均为+3价，但Y作为稀土副族元素，其独特的4f电子构型使Y₂O₃载体具有更丰富的氧空位和更强的电子给体能力，显著促进了活性Co²⁺物种的形成和分散；虽然Al₂O₃具有更高的比表面积和热稳定性，但主族元素Al与Co形成的CoAl₂O₄尖晶石相活性较低；10Co/Y₂O₃在700 ℃时氨转化率达100%，单位比表面积活性为10Co/Al₂O₃的3.2倍。研究结果为基于元素周期律的理性设计催化剂提供了新思路。

关键词: 氨分解, Co基催化剂, 载体效应, Y₂O₃, 主副族元素

Abstract:

Hydrogen production via ammonia decomposition is a crucial pathway toward achieving a "carbon-neutral society", and its catalytic efficiency is significantly influenced by the regulation of support materials. Based on the similar electronic structures of Al and Y elements, which belong to the main group and the subgroup (transition metal group) respectively, the differentiation mechanisms of Y?O? and Al?O? supports in cobalt-based catalysts were systematically compared.Catalyst characterization was performed using XRD, BET, SEM, XPS, H₂-TPR, and NH₃-TPD. The results show that although both Al and Y are trivalent, Y, as a rare-earth transition element, possesses a unique 4f electron configuration, which endows Y₂O₃ with richer oxygen vacancies and stronger electron-donating ability, significantly promoting the formation and dispersion of active Co²⁺ species. The 10Co/Y₂O₃ catalyst achieves an ammonia conversion of 100% at 700 ℃, and its specific surface area activity is 3.2 times that of 10Co/Al₂O₃. Although Al₂O₃ exhibits higher specific surface area and thermal stability, the spinel phase CoAl₂O₄ formed between the main-group element Al and Co shows low activity. This study provided new insights for the rational design of catalysts based on the periodic law.

Key words: Ammonia decomposition, Cobalt-based catalyst, Support effect, Y₂O₃, Main and subgroup elements

中图分类号:

TQ032.4

曹艺茹, 许慧琳, 李建宇, 金莹莹, 罗燕, 陈洪锋, 陈勇, 刘雪松. Y₂O₃与Al₂O₃负载钴催化剂的氨分解性能差异机理研究[J]. 石油化工高等学校学报, 2026, 39(4): 13-21.

Yiru CAO, Huilin XU, Jianyu LI, Yingying JIN, Yan LUO, Hongfeng CHEN, Yong CHEN, Xuesong LIU. Mechanism Study on the Difference in Ammonia Decomposition Performance between Co Catalysts Supported on Y₂O₃ and Al₂O₃[J]. Journal of Petrochemical Universities, 2026, 39(4): 13-21.

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链接本文: https://journal.lnpu.edu.cn/syhg/CN/10.12422/j.issn.1006-396X.2026.04.002

https://journal.lnpu.edu.cn/syhg/CN/Y2026/V39/I4/13

图/表 11

图1 老化前后催化剂的氨转化率随温度的变化曲线

Fig.1 Ammonia conversion rate curves of the catalyst before and after aging as a function of temperature

图2 氧化物及老化前后催化剂的XRD谱图

Fig.2 XRD spectra of oxides and catalysts before and after aging

表1 老化前后10Co/Y2O3的晶胞参数、晶胞体积和平均晶粒尺寸

Table 1 Cell parameters, cell volume and average grain size of 10Co/Y2O3 before and after aging

催化剂

晶胞参数/nm

晶胞体积/nm³

平均晶粒

尺寸/nm

10Co/Y₂O₃

10Co/Y₂O₃-A

图3 催化剂的SEM图

Fig.3 SEM image of the catalyst

表2 催化剂及载体的BET比表面积

Table 2 BET specific surface area of catalysts and carriers

催化剂及载体	BET比表面积/（m²·g^-1）
10Co/Al₂O₃	142.5
10Co/Y₂O₃	36.1
10Co/Y₂O₃-A	4.6
Al₂O₃	126.5
Y₂O₃	82.2

图4 氧化物及老化前后催化剂的Raman谱图

Fig.4 Raman spectra of oxides and catalysts before and after aging

图5 催化剂的XPS谱图

Fig.5 XPS spectra of the catalysts

图6 老化前后催化剂的H2-TPR曲线

Fig.6 H2-TPR curves of catalysts before and after aging

图7 老化前后催化剂的H2消耗量图

Fig.7 H2 consumption chart of catalyst before and after aging

图8 老化前后催化剂的NH3-TPD曲线after aging

Fig.8 NH3-TPD curves for catalysts before and

图9 老化前后催化剂的NH3脱附量after aging

Fig.9 NH3 desorption from catalysts before and

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Y₂O₃与Al₂O₃负载钴催化剂的氨分解性能差异机理研究

Mechanism Study on the Difference in Ammonia Decomposition Performance between Co Catalysts Supported on Y₂O₃ and Al₂O₃

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