• •
王龙龙1,2(), 秦志峰1,2(
), 班红艳1,2, 李乃珍1,2, 杜朕屹1,2, 于峰2, 翟志强3, 吴琼笑4
收稿日期:
2024-03-04
修回日期:
2024-06-18
出版日期:
2024-07-08
通讯作者:
秦志峰
作者简介:
王龙龙(1999—),男,硕士研究生, 15383414720@163.com
基金资助:
Longlong WANG1,2(), Zhifeng QIN1,2(
), Hongyan BAN1,2, Naizhen LI1,2, Zhenyi DU1,2, Feng YU2, Zhiqiang ZHAI3, Qiongxiao WU4
Received:
2024-03-04
Revised:
2024-06-18
Online:
2024-07-08
Contact:
Zhifeng QIN
摘要:
探讨了Al2O3载体孔结构对FeMo/Al2O3预加氢脱硫(HDS)催化剂活性和选择性的影响,采用浸渍法成功制备了一系列具有不同孔结构的FeMo/Al2O3催化剂,并通过微型固定床技术对其在模拟焦炉煤气中COS、CS2、C4H4S和C2H4的HDS活性和选择性进行了系统评价,通过N2吸附-脱附、红外碳硫、XRD、NH3-TPD、H2-TPR、XPS、Raman以及HRTEM等技术对催化剂进行了表征。研究结果揭示了Al2O3载体孔结构对催化剂活性相MoS2有显著影响,从而影响加氢脱硫活性和选择性,其中较大孔径的载体更有利于COS和CS2的有效转化,而较小孔径的载体则更倾向于促进C4H4S和C2H4的转化;此外,具有较大孔径的催化剂不仅展现出更低的积碳倾向,还通过提高Mo物种的分散性,有效调控了MoS2片晶的生长尺寸和层数,从而在COS和CS2的加氢脱硫活性上实现了优异性能,这些发现为高效HDS催化剂的设计与开发开辟了新途径。
中图分类号:
王龙龙, 秦志峰, 班红艳, 李乃珍, 杜朕屹, 于峰, 翟志强, 吴琼笑. Al2O3载体孔结构优化:提升FeMo/Al2O3催化剂在焦炉煤气加氢脱硫性能[J]. 化工学报, DOI: 10.11949/0438-1157.20240259.
Longlong WANG, Zhifeng QIN, Hongyan BAN, Naizhen LI, Zhenyi DU, Feng YU, Zhiqiang ZHAI, Qiongxiao WU. Optimization of Al2O3 support pore structure: enhancing the hydrodesulfurization performance of FeMo/Al2O3 catalyst in coke oven gas[J]. CIESC Journal, DOI: 10.11949/0438-1157.20240259.
样品 | 孔体积(cm3·g-1) | 比表面积(m2·g-1) | 平均孔径(nm) | 吸水率(ml·g-1) |
---|---|---|---|---|
a-Al2O3载体 | 0.86 | 246.4 | 12.4 | 129.41 |
b-Al2O3载体 | 0.78 | 285.8 | 10.2 | 148.91 |
c-Al2O3载体 | 0.65 | 263.2 | 9.6 | 107.53 |
d-Al2O3载体 | 0.62 | 214.2 | 8.8 | 116.30 |
e-Al2O3载体 | 0.49 | 254.7 | 8.2 | 70.33 |
表1 Al2O3载体孔结构参数和吸水率
Table 1 Pore structure parameters and the water absorption of the Al2O3 supports
样品 | 孔体积(cm3·g-1) | 比表面积(m2·g-1) | 平均孔径(nm) | 吸水率(ml·g-1) |
---|---|---|---|---|
a-Al2O3载体 | 0.86 | 246.4 | 12.4 | 129.41 |
b-Al2O3载体 | 0.78 | 285.8 | 10.2 | 148.91 |
c-Al2O3载体 | 0.65 | 263.2 | 9.6 | 107.53 |
d-Al2O3载体 | 0.62 | 214.2 | 8.8 | 116.30 |
e-Al2O3载体 | 0.49 | 254.7 | 8.2 | 70.33 |
气体名称 | 纯度或含量 | 平衡气体 |
---|---|---|
乙烯 | 99.9 % | ----- |
氮气 | 99.99 % | ----- |
预硫化气体 | H2S ~ 3% | H2 |
含硫反应气体 | COS ~ 170.86mg/m3、CS2 ~ 130.53mg/m3、C4H4S~ 18.45mg/m3 | H2 |
硫化物标气 | H2S ~ 204.95mg/m3、COS ~ 222.22mg/m3、CH3SH ~ 142.07mg/m3、C2H5SH~ 140.91mg/m3、CH3SCH3 ~ 146.19mg/m3、CS2 ~ 224.54mg/m3、C4H4S ~ 210.93mg/m3、 CH3S2CH3 ~ 212.46mg/m3、C2H5SCH3 ~ 209.91mg/m3、(C2H5)S ~ 209.42mg/m3 | N2 |
表2 实验所用气体组分和纯度
Table 2 Test gas composition and concentration
气体名称 | 纯度或含量 | 平衡气体 |
---|---|---|
乙烯 | 99.9 % | ----- |
氮气 | 99.99 % | ----- |
预硫化气体 | H2S ~ 3% | H2 |
含硫反应气体 | COS ~ 170.86mg/m3、CS2 ~ 130.53mg/m3、C4H4S~ 18.45mg/m3 | H2 |
硫化物标气 | H2S ~ 204.95mg/m3、COS ~ 222.22mg/m3、CH3SH ~ 142.07mg/m3、C2H5SH~ 140.91mg/m3、CH3SCH3 ~ 146.19mg/m3、CS2 ~ 224.54mg/m3、C4H4S ~ 210.93mg/m3、 CH3S2CH3 ~ 212.46mg/m3、C2H5SCH3 ~ 209.91mg/m3、(C2H5)S ~ 209.42mg/m3 | N2 |
图1 不同孔结构载体FeMo/Al2O3催化剂HDS活性(反应条件:压力为1.0 MPa,空速为5400 h-1(含硫反应气体与C2H4体积比为5:1);a:FeMo/a-Al2O3催化剂,b:FeMo/b-Al2O3催化剂,c:FeMo/c-Al2O3催化剂,d:FeMo/d-Al2O3催化剂,e:FeMo/e-Al2O3催化剂,下同)
Fig.1 HDS performance of FeMo/Al2O3 catalysts of different support pore structures
图2 不同孔结构载体FeMo/Al2O3催化剂加氢产物分布(反应条件:压力为1.0 MPa,空速为5400 h-1(含硫反应气体与C2H4体积比为5:1))
Fig. 2 HDS reaction product composition of FeMo/Al2O3 catalyst at different support pore structures
催化剂样品 | 比表面积(m2·g-1) | 孔体积(cm3·g-1) | 平均孔径(nm) | 碳含量(wt.%) | 硫含量(wt.%) | |
---|---|---|---|---|---|---|
FeMo/a-Al2O3 | 新鲜催化剂 | 226.3 | 0.82 | 13.1 | 0.03 | 0.36 |
反应后催化剂 | 210.6 | 0.81 | 13.6 | 0.37 | 3.41 | |
FeMo/b-Al2O3 | 新鲜催化剂 | 276.1 | 0.72 | 10.7 | 0.03 | 0.20 |
反应后催化剂 | 227.2 | 0.65 | 11.1 | 0.48 | 3.08 | |
FeMo/c-Al2O3 | 新鲜催化剂 | 218.6 | 0.61 | 10.3 | 0.03 | 0.21 |
反应后催化剂 | 200.9 | 0.59 | 10.7 | 1.07 | 3.37 | |
FeMo/d-Al2O3 | 新鲜催化剂 | 207.4 | 0.60 | 10.2 | 0.04 | 0.23 |
反应后催化剂 | 170.2 | 0.56 | 10.8 | 1.04 | 3.46 | |
FeMo/e-Al2O3 | 新鲜催化剂 | 221.8 | 0.45 | 8.6 | 0.02 | 0.21 |
反应后催化剂 | 194.3 | 0.41 | 8.9 | 1.06 | 2.87 |
表3 不同孔结构载体FeMo/c-Al2O3催化剂反应前后物理性能
Table 3 Textural properties of the before and after the reaction samples at different support
催化剂样品 | 比表面积(m2·g-1) | 孔体积(cm3·g-1) | 平均孔径(nm) | 碳含量(wt.%) | 硫含量(wt.%) | |
---|---|---|---|---|---|---|
FeMo/a-Al2O3 | 新鲜催化剂 | 226.3 | 0.82 | 13.1 | 0.03 | 0.36 |
反应后催化剂 | 210.6 | 0.81 | 13.6 | 0.37 | 3.41 | |
FeMo/b-Al2O3 | 新鲜催化剂 | 276.1 | 0.72 | 10.7 | 0.03 | 0.20 |
反应后催化剂 | 227.2 | 0.65 | 11.1 | 0.48 | 3.08 | |
FeMo/c-Al2O3 | 新鲜催化剂 | 218.6 | 0.61 | 10.3 | 0.03 | 0.21 |
反应后催化剂 | 200.9 | 0.59 | 10.7 | 1.07 | 3.37 | |
FeMo/d-Al2O3 | 新鲜催化剂 | 207.4 | 0.60 | 10.2 | 0.04 | 0.23 |
反应后催化剂 | 170.2 | 0.56 | 10.8 | 1.04 | 3.46 | |
FeMo/e-Al2O3 | 新鲜催化剂 | 221.8 | 0.45 | 8.6 | 0.02 | 0.21 |
反应后催化剂 | 194.3 | 0.41 | 8.9 | 1.06 | 2.87 |
反应后催化剂 | Mo4+ | Mo5+ | Mo6+ | SMo | |||
---|---|---|---|---|---|---|---|
ar.%1(229.0eV) | ar.%(232.2eV) | ar.%(230.5eV) | ar.%(233.6eV) | ar.%(233.5eV) | ar.%(236.2eV) | ||
FeMo/a-Al2O3 | 29 | 25 | 8 | 1 | 21 | 17 | 54 |
FeMo/b-Al2O3 | 21 | 25 | 7 | 6 | 20 | 21 | 46 |
FeMo/c-Al2O3 | 15 | 28 | 4 | 6 | 20 | 17 | 43 |
FeMo/d-Al2O3 | 15 | 27 | 14 | 4 | 19 | 22 | 42 |
FeMo/e-Al2O3 | 20 | 19 | 7 | 3 | 30 | 21 | 40 |
表4 反应后催化剂XPS表面元素含量
Table 4 Surface compositions calculated from XPS spectra for Mo and S elements in catalysts after reaction
反应后催化剂 | Mo4+ | Mo5+ | Mo6+ | SMo | |||
---|---|---|---|---|---|---|---|
ar.%1(229.0eV) | ar.%(232.2eV) | ar.%(230.5eV) | ar.%(233.6eV) | ar.%(233.5eV) | ar.%(236.2eV) | ||
FeMo/a-Al2O3 | 29 | 25 | 8 | 1 | 21 | 17 | 54 |
FeMo/b-Al2O3 | 21 | 25 | 7 | 6 | 20 | 21 | 46 |
FeMo/c-Al2O3 | 15 | 28 | 4 | 6 | 20 | 17 | 43 |
FeMo/d-Al2O3 | 15 | 27 | 14 | 4 | 19 | 22 | 42 |
FeMo/e-Al2O3 | 20 | 19 | 7 | 3 | 30 | 21 | 40 |
反应后催化剂 | 平均堆叠层数 | 平均片晶长度/nm |
---|---|---|
FeMo/a-Al2O3 | 2.56 | 4.52 |
FeMo/b-Al2O3 | 2.75 | 4.72 |
FeMo/c-Al2O3 | 3.31 | 8.56 |
FeMo/d-Al2O3 | 5.25 | 9.4 |
FeMo/e-Al2O3 | 8.28 | 10.88 |
表5 反应后催化剂TEM统计结果
Table 5 TEM statistical results in catalysts after reaction
反应后催化剂 | 平均堆叠层数 | 平均片晶长度/nm |
---|---|---|
FeMo/a-Al2O3 | 2.56 | 4.52 |
FeMo/b-Al2O3 | 2.75 | 4.72 |
FeMo/c-Al2O3 | 3.31 | 8.56 |
FeMo/d-Al2O3 | 5.25 | 9.4 |
FeMo/e-Al2O3 | 8.28 | 10.88 |
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