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Performance study of Mn2O3@SiO2 oxygen carrier for chemical looping oxidative dehydrogenation of ethane to ethylene
- Low-Carbon Chemistry and Chemical Engineering Vol. 50, Issue 8, Pages: 133-143(2025)
- 作者机构：
1.西安交通大学 化学工程与技术学院，陕西 西安 710049
2.中石化安全工程研究院有限公司 化学品安全全国重点实验室，山东 青岛 266071
- 作者简介：
- 基金信息：
DOI：10.12434/j.issn.2097-2547.20250078
CLC： TQ032Received：28 February 2025，
Revised：07 April 2025，
Published：25 August 2025
- 稿件说明：
移动端阅览
王智超,梁威,刘根等.Mn2O3@SiO2载氧体用于乙烷化学链氧化脱氢制乙烯性能研究[J].低碳化学与化工,2025,50(8):133-143.
WANG Zhichao,LIANG Wei,LIU Gen,et al.Performance study of Mn2O3@SiO2 oxygen carrier for chemical looping oxidative dehydrogenation of ethane to ethylene[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(8):133-143.
王智超,梁威,刘根等.Mn2O3@SiO2载氧体用于乙烷化学链氧化脱氢制乙烯性能研究[J].低碳化学与化工,2025,50(8):133-143. DOI： 10.12434/j.issn.2097-2547.20250078.
WANG Zhichao,LIANG Wei,LIU Gen,et al.Performance study of Mn2O3@SiO2 oxygen carrier for chemical looping oxidative dehydrogenation of ethane to ethylene[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(8):133-143. DOI： 10.12434/j.issn.2097-2547.20250078.
摘要
乙烷化学链氧化脱氢（Chemical looping oxidative dehydrogenation，CL-ODH）是一种利用载氧体的晶格氧将乙烷转化为乙烯的绿色高效过程。然而，该过程往往面临反应活性或乙烯选择性难以兼顾的问题，导致乙烷转化率或乙烯选择性较低。提出了SiO
2
包覆Mn
2
O
3
载氧体的设计策略，合成了具有不同
n
(Mn)/
n
(Si)的Mn
2
O
3
@SiO
2
载氧体。采用XRD、N
2
物理吸/脱附、H
2
-TPR和XPS等方法，对载氧体的晶相结构、织构性质、还原性能和表面物种化学状态等进行了表征。结果表明，SiO
2
在Mn
2
O
3
表面形成包覆层，有助于优化载氧体的孔结构，增大载氧体的比表面积，减小Mn
2
O
3
晶粒尺寸，提高其分散性，从而提升反应活性。同时，SiO
2
的引入增大了近表面Mn—O结合能，减小了晶格氧的释放速率，减小了表面非选择性氧物种含量，显著提升了乙烯选择性。在700 ℃、20%C
2
H
6
/80%Ar（50 mL/min）和反应时间2 min条件下，
n
(Mn)/
n
(Si)为0.9的Mn
2
O
3
@SiO
2
载氧体作用下，乙烷转化率达42.8%，乙烯选择性达73.4%。
Abstract
Chemical looping oxidative dehydrogenation (CL-ODH) of ethane is a green and efficient process that uses lattice oxygen of oxygen carrier to convert ethane into ethylene. However
this process often faces the problem that the reaction activity or ethylene selectivity is difficult to balance
resulting in low ethane conversion rate or ethylene selectivity. A design strategy of SiO
2
coated Mn
2
O
3
oxygen carriers was proposed
and Mn
2
O
3
@SiO
2
oxygen carriers with different
n
(Mn)/
n
(Si) were synthesized. XRD
N
2
physical absorption/desorption
H
2
-TPR and XPS were used to characterize the crystal structures
textural properties
reduction properties and surface species chemical states of the oxygen carriers. The results show that SiO
2
forms a coating layer on the surface of Mn
2
O
3
which can optimize the pore structure and increase the specific surface area of oxygen carriers
reduce the grain size of Mn
2
O
3
improve the dispersion
and thus improve the reaction activity. At the same time
the introduction of SiO
2
enhances the near-surface Mn—O binding energy
reduces the release rate of lattice oxygen
reduces the content of non-selective oxygen species on the surface and significantly improves the ethylene selectivity. Under the conditions of 700 ℃
20%C
2
H
6
/80%Ar (50 mL/min)
reaction time of 2 min
with the Mn
2
O
3
@SiO
2
oxygen carrier (
n
(Mn)/
n
(Si) is 0.9)
ethane conversion achieves 42.8% and ethylene selectivity achieves 73.4%.
关键词
Keywords
references
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