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1.浙江海洋大学 全省临港石化污染控制重点实验室,浙江 舟山 316022
2.浙江海洋大学 临港石油天然气储运技术国家地方联合工程研究中心,浙江 舟山 316022
黄礼智(1999—),硕士研究生,研究方向为Ni基催化剂开发应用,E-mail:huanglizhi@zjou.edu.cn。
王路辉(1981—),博士,教授,研究方向为能源与环境催化,E-mail:wangluhui1008@zjou.edu.cn。
收稿:2025-01-05,
修回:2025-01-25,
纸质出版:2025-10-25
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黄礼智,刘亚丽,魏勤洪等.三维介孔Ni-ZrO2催化剂甲烷干重整性能研究[J].低碳化学与化工,2025,50(10):19-26.
HUANG Lizhi,LIU Yali,WEI Qinhong,et al.Performance study of dry reforming of methane over three-dimensional mesoporous Ni-ZrO2 catalysts[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(10):19-26.
黄礼智,刘亚丽,魏勤洪等.三维介孔Ni-ZrO2催化剂甲烷干重整性能研究[J].低碳化学与化工,2025,50(10):19-26. DOI: 10.12434/j.issn.2097-2547.20250005.
HUANG Lizhi,LIU Yali,WEI Qinhong,et al.Performance study of dry reforming of methane over three-dimensional mesoporous Ni-ZrO2 catalysts[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(10):19-26. DOI: 10.12434/j.issn.2097-2547.20250005.
甲烷干重整(DRM)反应能够将CO
2
和CH
4
两种主要温室气体高效转化为H
2
和CO,从而实现资源化利用,具有重要的研究意义。Ni基催化剂因具有成本较低和活性较高的特点备受关注,但易因积炭导致失活,这一问题亟待解决。采用硅溶胶辅助溶液燃烧法制备了具有三维介孔结构的Ni-ZrO
2
催化剂,并将其应用于低温DRM反应。通过N
2
吸/脱附、XRD、H
2
-TPR、TEM和TG-DTA等多种表征手段,系统研究了催化剂结构以及Ni含量(质量分数,下同)和反应温度对催化剂催化性能的影响,并与普通浸渍法及传统溶液燃烧法制备的催化剂进行了对比。结果表明,硅溶胶辅助溶液燃烧法制备的催化剂具有较大的比表面积和稳定的三维介孔结构,并展现出更强的金属-载体相互作用。在催化性能方面,Ni含量对催化剂抗积炭性能和催化活性均具有显著影响。随着Ni含量的增大,催化剂的积炭倾向显著增强。在温度为600 °C、空速为135000 mL/(g·h)下进行20 h低温DRM反应后,具有三维介孔结构的1%Ni-ZrO
2
-CSC催化剂的CH
4
和CO
2
转化率分别维持在31%和38%,
n
(H
2
)/
n
(CO)稳定在0.45,且未观察到积炭生成,表明其具有优异的抗积炭性能。
The dry reforming of methane (DRM) reaction efficiently converts two major greenhouse gases
CO
2
and CH
4
into H
2
and CO
thereby achieving resource utilization and holding significant research value. Ni-based catalysts have garnere
d attention due to their low cost and high activity
but their deactivation caused by coking remains a pressing issue. Three-dimensional mesoporous Ni-ZrO
2
catalysts were prepared by colloidal silica-assisted solution combustion method and applied to low-temperature DRM reaction. Characterizations including N
2
adsorption/desorption
XRD
H
2
-TPR
TEM
and TG-DTA were conducted to systematically investigate the structures and the effects of Ni contents (mass fraction
the same below) and reaction temperatures on catalytic performance of catalysts. Comparisons were made with catalysts prepared via ordinary impregnation method and traditional solution combustion method. The results indicate that the catalysts prepared by colloidal silica-assisted solution combustion method exhibit larger specific surface areas
stable three-dimensional mesoporous structures
and have strong metal-support interactions. Regarding catalytic performance
Ni contents significantly affect both anti-coking performances and catalytic activities. As the Ni contents increase
the tendency of catalysts for coking becomes more pronounced. After a 20 h low-temperature DRM reaction at the temperature of 600 ℃ and space velocity of 135000 mL/(g·h)
the three-dimensional mesoporous 1%Ni-ZrO
2
-CSC catalyst maintains CH
4
and CO
2
conversion rates of 31% and 38%
respectively. The
n
(H
2
)/
n
(CO) stabilizes at 0.45
and no coking is observed
demonstrating 1%Ni-ZrO
2
-CSC’s excellent resistance to coking.
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