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Study on catalytic performance of mesoporous chromium/cerium-zirconium oxide system for CO2-oxidative propane dehydrogenation to propylene
- Low-Carbon Chemistry and Chemical Engineering Vol. 50, Issue 5, Pages: 40-48(2025)
- 作者机构：
中石化石油化工科学研究院有限公司，北京 100083
- 作者简介：
- 基金信息：
DOI：10.12434/j.issn.2097-2547.20240261
CLC： TQ426.6Received：14 June 2024，
Revised：16 July 2024，
Published：25 May 2025
- 稿件说明：
移动端阅览
陈晓昂,张荣俊,徐润等.介孔铬/铈锆氧化物体系催化CO2氧化丙烷脱氢制丙烯反应性能研究[J].低碳化学与化工,2025,50(05):40-48.
CHEN Xiaoang,ZHANG Rongjun,XU Run,et al.Study on catalytic performance of mesoporous chromium/cerium-zirconium oxide system for CO2-oxidative propane dehydrogenation to propylene[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(05):40-48.
陈晓昂,张荣俊,徐润等.介孔铬/铈锆氧化物体系催化CO2氧化丙烷脱氢制丙烯反应性能研究[J].低碳化学与化工,2025,50(05):40-48. DOI： 10.12434/j.issn.2097-2547.20240261.
CHEN Xiaoang,ZHANG Rongjun,XU Run,et al.Study on catalytic performance of mesoporous chromium/cerium-zirconium oxide system for CO2-oxidative propane dehydrogenation to propylene[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(05):40-48. DOI： 10.12434/j.issn.2097-2547.20240261.
摘要
丙烷脱氢（PDH）制丙烯是较为经济的制丙烯工艺之一，然而丙烷脱氢制丙烯存在丙烷单程转化率较低、催化剂中Cr负载量较高污染环境等问题。通过蒸发诱导自组装法合成了一系列不同
n
(Ce):
n
(Zr)铈锆氧化物，然后采用等体积浸渍法负载Cr制备了相应的催化剂，并选用CO
2
氧化丙烷脱氢（CO
2
-OPDH）法制备丙烯。通过XRD、N
2
吸/脱附、SEM、TEM和XPS等对催化剂进行了表征。结果表明，所有催化剂均形成了均一的铈锆固溶体，催化剂比表面积大于70 m
2
/g，存在介孔结构；随着
n
(Ce):
n
(Zr)减小，催化剂中
n
(Cr
3+
):(
n
(Cr
3+
) +
n
(Cr
6+
))逐渐增大，有利于提高其催化性能。所有催化剂均具有较高的丙烷初始转化率和丙烯选择性，在600 ℃、0.1 MPa和丙烷空速200 h
-1
的条件下，
n
(Ce):
n
(Zr) = 1:9的催化剂的丙烷初始转化率达到53%，反应稳定后丙烯选择性接近90%；而后随着
n
(Ce):
n
(Zr)增大，丙烷初始转化率逐渐降低。当
n
(Ce):
n
(Zr) = 5:5时，催化剂的丙烷初始转化率与工业剂相近。再生循环测试表明
n
(Ce):
n
(Zr) = 1:9时催化剂具有较好的再生稳定性，这也为后续低Cr负载量丙烷脱氢催化剂的开发提供了参考和借鉴。
Abstract
Propane dehydrogenation (PDH) to propylene is an economical process. However
PDH faces challenges including low propane conversion and high Cr loading capacity in the catalyst
which contributes the environment pollution. To address these issues
a series of cerium-zirconium oxides with
n
(Ce):
n
(Zr) were synthesized by evaporation-induced self-assembly
and the corresponding catalysts were prepared by equal volume impregnation method and loaded with Cr
and CO
2
oxidative dehydrogenation of propane (CO
2
-OPDH) was explored as an alternative route for propylene production. The catalysts were characterized by XRD
N
2
adsorption/desorption
SEM
TEM and XPS. The results show that all catalysts form homogeneous cerium-zirconium solid solution with specific surface areas exceeding 70 m
2
/g and mesoporous structure. With the decrease of
n
(Ce):
n
(Zr)
n
(Cr
3+
):(
n
(Cr
3+
) +
n
(Cr
6+
) in the catalyst gradually increases
which enhances its catalytic performance. All catalysts have high initial propane conversion rate and propylene selectivity. With the increase of
n
(Ce):
n
(Zr)
the initial conversion rate of propane decreases gradually. The catalyst with
n
(Ce):
n
(Zr) of 1:9 exhibits initial propane conversi
on of 53% and propylene selectivity (when the reaction reaches stability ) close to 90% at 600 ℃
0.1 MPa and propane space velocity of 200 h
-1
. The catalyst with
n
(Ce):
n
(Zr) of 5:5 achieves a propane initial conversion rate comparable to that of industrial catalysts. Regeneration cycle test reveals that the catalyst with
n
(Ce):
n
(Zr) = 1:9 exhibits good stability
which provides valuable insights for the development of low-Cr loading capacity propane dehydrogenation catalysts. .
关键词
Keywords
references
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