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NiO含量对NiMo/Al2O3催化剂在焦炉煤气中噻吩加氢脱硫性能的影响
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- 低碳化学与化工 2025, 50(4): 71-79.
- 作者机构：
1.太原理工大学 省部共建煤基能源清洁高效利用国家重点实验室，山西 太原 030024
2.太原理工大学 化学工程与技术学院，山西 太原 030024
3.山西东义煤电铝集团煤化工有限公司，山西 孝义 032200
4.东莞市能源投资集团有限公司，广东 东莞 523000
- 作者简介：
李姣姣（1997—），硕士研究生，研究方向为气体净化与工业催化，E-mail：1832045258@qq.com。
秦志峰（1983—），博士，副教授，硕士研究生导师，研究方向为煤转化过程中污染物控制及治理，E-mail：qinzhifeng2022@163.com。
- 基金信息：山西省科技重大专项(MJH2016-03);山西浙大新材料与化工研究院研发项目(2021ST-AT-002);东莞市能源投资集团有限公司攻关项目(RH2000004464)
DOI：10.12434/j.issn.2097-2547.20240231
中图分类号： TQ426收稿日期：2024-05-24，
修回日期：2024-08-02，
纸质出版日期：2025-04-25
- 稿件说明：
移动端阅览
李姣姣,秦志峰,李晓红等.NiO含量对NiMo/Al2O3催化剂在焦炉煤气中噻吩加氢脱硫性能的影响[J].低碳化学与化工,2025,50(04):71-79.
LI Jiaojiao,QIN Zhifeng,LI Xiaohong,et al.Effect of NiO content on thiophene hydrodesulfurization performance of NiMo/Al2O3 catalyst in coke oven gas[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(04):71-79.
李姣姣,秦志峰,李晓红等.NiO含量对NiMo/Al2O3催化剂在焦炉煤气中噻吩加氢脱硫性能的影响[J].低碳化学与化工,2025,50(04):71-79. DOI： 10.12434/j.issn.2097-2547.20240231.
LI Jiaojiao,QIN Zhifeng,LI Xiaohong,et al.Effect of NiO content on thiophene hydrodesulfurization performance of NiMo/Al2O3 catalyst in coke oven gas[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(04):71-79. DOI： 10.12434/j.issn.2097-2547.20240231.
摘要
焦炉煤气作为气体资源，常被用作化工原料，然而其中噻吩（C
4
H
4
S）等硫化物杂质的存在对催化剂具有较强毒害作用，工业上常通过二级镍钼加氢脱硫对噻吩进行深度脱除。为探究金属负载量对催化剂性能的影响，采用浸渍法制备了不同NiO含量（5%、10%、15%和20%，质量分数）的NiMo/Al
2
O
3
催化剂；在反应温度250~390 ℃、压力1 MPa和原料空速4500 h
-1
条件下，对催化剂焦炉煤气噻吩加氢脱硫性能进行了测试；并通过N
2
吸/脱附、XRD、H
2
-TPR和XPS等表征手段，探究了NiO含量对NiMo/Al
2
O
3
催化剂性能的影响。结果表明，在270~370 ℃区间内，催化剂的C
4
H
4
S转化率从大到小依次为Ni
5
Mo
15
/Al
2
O
3
、Ni
10
Mo
15
/Al
2
O
3
、Ni
15
Mo
15
/Al
2
O
3
和Ni
20
Mo
15
/Al
2
O
3
。其中，Ni
5
Mo
15
/Al
2
O
3
催化剂，290 ℃时C
4
H
4
S转化率达到70%，330 ℃时达到90%，明显高于其他3种催化剂。这归因于该催化剂在预硫化过程中，生成了更多活性物种MoS
2
，硫化程度较高。但随着NiO含量增大，可能发生NiO包覆MoO
3
的现象，导致催化剂硫化程度下降，催化性能减弱。
Abstract
Coke oven gas
as a valuable gaseous resource
is often used as a chemical raw material. However
sulfur impurities such as thiophene (C
4
H
4
S) in the gas exhibit strong poisoning effects on catalysts. Industrially
deep removal of thiophene is typically achieved via secondary Ni-Mo hydrodesulfurization. To investigate the effect of metal loading on catalyst performance
NiMo/Al
2
O
3
catalysts with varying NiO contents (5%
10%
15% and 20%
mass fraction) were prepared using the impregnation method. The hydrodesulfurization performance of these catalysts in coke oven gas was tested under conditions of reaction temperatures from 250 ℃ to 390 ℃
the pressure of 1 MPa
and the gas hourly space velocity of 4500 h
-1
. The effects of NiO content on the catalyst performance were analyzed using characterization techniques such as N
2
adsorption/desorption
XRD
H
2
-TPR
and XPS. The results show that in the temperature range of 270 ℃ to 370 ℃
the C
4
H
4
S conversion rates of the catalysts decrease in the order of Ni
5
Mo
15
/Al
2
O
3
Ni
10
Mo
15
/Al
2
O
3
Ni
15
Mo
15
/Al
2
O
3
and Ni
20
Mo
15
/Al
2
O
3
. Among them
the Ni
5
Mo
15
/Al
2
O
3
catalyst achieves a C
4
H
4
S conversion rate of 70% at 290 ℃ and 90% at 330 ℃
significantly outperforming the other three catalysts. This is attributed to the formation of more active MoS
2
species during the presulfurization process
resulting in a higher degree of sulfuration. However
with increasing NiO content
the phenomenon of NiO encapsulating MoO
3
likely occurres
resulting in decreased sulfuration and diminished catalytic performance.
关键词
Keywords
references
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