离子交换法制备Pt-Sn<sub>E</sub>/Mg (Al) O催化剂及其烷烃催化脱氢性能

陈领鹏; 田志鹏; 吕微; 司展; 刘琪英; 定明月; 陈伦刚; 马隆龙; 张琦; 王铁军; 王晨光

离子交换法制备Pt-Sn_E/Mg (Al) O催化剂及其烷烃催化脱氢性能

陈领鹏^{1, 2},
田志鹏^{1, 2},
吕微¹,
司展³,
刘琪英¹,
定明月¹,
陈伦刚¹,
马隆龙¹,
张琦¹,
王铁军¹,
王晨光^1, ,

1.
中国科学院广州能源研究所可再生能源重点实验室, 广东广州 510640
2.
中国科学院大学, 北京 100049
3.
中国农业大学生物质能源工程与低碳技术研究室, 北京 100083

基金项目:

国家自然科学基金 51476175

中国科学院百人计划 y507y51001

详细信息

通讯作者:
王晨光, Tel: 020-37029721, E-mai: wangcg@ms.giec.ac.cn

中图分类号: O643
计量
- 文章访问数: 72
- HTML全文浏览量: 23
- PDF下载量: 7
- 被引次数: 0
出版历程
- 收稿日期: 2015-12-16
- 修回日期: 2016-03-01
- 网络出版日期: 2021-01-23
- 刊出日期: 2016-05-10

Preparation of Pt-Sn_E/Mg (Al) O catalyst by anion exchange method and its performance in alkane dehydrogenation

1.
Key Laboratory of Renewable Energy, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
Bio Energy Engineering and Low Carbon Technology Laboratory, China Agricultural University, Beijing 100083, China

Funds:

the National Natural Science Foundation of China 51476175

the Hundred Talents Program of the Chinese Academy of Sciences y507y51001

摘要

摘要: 以水滑石为载体, 采用离子交换法制备了Pt-Sn_E/Mg (Al) O催化剂, 并对其进行了X射线衍射、N₂物理吸附、透射电镜等技术表征; 考察了该离子交换法制备的Pt-Sn_E/Mg (Al) O催化剂对乙烷和丙烷脱氢的催化性能, 并与浸渍法制备的Pt-Sn_I/Mg (Al) O催化剂进行了比较。结果表明, 利用离子交换法制备的Pt-Sn_E/Mg (Al) O催化剂其反应活性和稳定性明显优于浸渍法制备Pt-Sn_I/Mg (Al) O催化剂的。在相同条件下反应2 h后, Pt-Sn_E/Mg (Al) O催化剂和Pt-Sn_I/Mg (Al) O催化剂的乙烷催化脱氢转化率分别为12.2%和3.1%, 丙烷催化脱氢转化率分别为38.7%和26.4%。
- 铂 /
- 水滑石 /
- Mg (Al) O /
- 离子交换 /
- 乙烷脱氢 /
- 丙烷脱氢
Abstract: Pt-Sn_E/Mg (Al) O catalyst was prepared by anion exchange method with hydrotalcite as the support. The Pt-Sn_E/Mg (Al) O catalyst was characterized by XRD, nitrogen sorption, CO-TPD and TEM; its catalytic performance in the dehydrogenation of ethane and propane was compared with that the Pt-Sn_I/Mg (Al) O catalyst obtained by impregnation method. The results indicate that under the same reaction conditions, the conversions of ethane over the Pt-Sn_E/Mg (Al) O and Pt-Sn_I/Mg (Al) O catalysts are 12.2% and 3.1%, respectively, whist the conversions of propane over these two catalysts are 38.7% and 26.4%, respectively. Such results illustrate that the Pt-Sn_E/Mg (Al) O catalyst prepared by the anion exchange method is obviously superior to the Pt-Sn_I/Mg (Al) O catalyst prepared by the impregnation method in terms of catalytic activity and stability for alkane dehydrogenation.
- platinum /
- hydrotalcite /
- Mg (Al) O /
- anion exchange /
- ethane dehydrogenation /
- propane dehydrogenation

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图 1 催化剂的XRD谱图

Figure 1 XRD patterns of the catalysts

a: Pt-Sn_I/Mg (Al) O; b: Pt-Sn_E/Mg (Al) O

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图 2 催化剂的TEM照片和颗粒粒径分布

Figure 2 EM images (a, b) and particle size distributions (a′, b′) of two catalysts

(a, a′): Pt-Sn_E/Mg (Al) O; (b, b′): Pt-Sn_I/Mg (Al) O

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图 3 催化剂的CO-TPD谱图

Figure 3 CO-TPD profiles of two catalysts

a: Pt-Sn_E/Mg (Al) O; b: Pt-Sn_I/Mg (Al) O

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图 4 催化剂的NH₃-TPD谱图

Figure 4 NH₃-TPD profiles of the catalysts

a:Mg (Al) O; b: Pt-Sn_I/Mg (Al) O; c: Pt-Sn_E/Mg (Al) O

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图 5 催化剂的H₂-TPD谱图

Figure 5 H₂-TPD profiles of two catalysts

a: Pt-Sn_E/Mg (Al) O; b: Pt-Sn_I/Mg (Al) O

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图 6 催化剂的Sn 3d_5/2 XPS谱图

Figure 6 Sn 3d_5/2 XPS profiles of the catalysts

(a): Pt-Sn_E/Mg (Al) O; (b): Pt-Sn_I/Mg (Al) O

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图 7 催化剂对乙烷催化脱氢性能随时间的变化

Figure 7 Ethane dehydrogenation over two catalysts versus time on stream

(a): ethane conversion; (b): ethene selectivity

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图 8 催化剂对丙烷催化脱氢性能随时间的变化

Figure 8 Propane dehydrogenation over two catalysts versus time on stream

(a): propane conversion; (b): propene selectivity

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图 9 Pt-Sn_E/Mg (Al) O催化剂对乙烷和丙烷混合气催化脱氢性能随时间变化

Figure 9 Dehydrogenation of ethane and propane mixture over the Pt-Sn_E/Mg (Al) O catalyst versus time on stream

(a): C₂H₆/C₃H₈ conversion; (b): CH_4/H₂ mole ratio

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图 10 Pt-Sn_E/Mg (Al) O催化剂对乙烷脱氢及反应丙烷脱氢反应的稳定性

Figure 10 Stability test of the Pt-Sn_E/Mg (Al) O catalyst in ethane dehydrogenation and propane dehydrogenation

(a): C₂H₆/C₃H₈ conversion; (b): C₂H₄/C₃H₆ selectivity

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图 11 反应后Pt-Sn_E/Mg (Al) O催化剂的TG-MS曲线

Figure 11 TG-MS curves of the used Pt-Sn_E/Mg (Al) O catalyst after dehydrogenation reaction

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表 1 催化剂BET比表面积和孔容

Table 1 BET surface area and pore volume of the Pt-Sn_E/Mg (Al) O and Pt-Sn_I/Mg (Al) O catalysts

Catalyst	Specific area A/(m²·g^-1)	Pore volume v/(cm³·g^-1)
Pt-Sn_I/Mg (Al) O	37.5	0.32
Pt-Sn_E/Mg (Al) O	84.8	0.54

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表 2 催化剂XPS结果

Table 2 XPS results of the Pt-Sn_E/Mg (Al) O and Pt-Sn_I/Mg (Al) O catalysts

Catalyst	Binding energy E/eV
Pt-Sn_E/Mg (Al) O	485.4(25.8%)	486.2(51.2%)	486.9(23.0%)
Pt-Sn_I/Mg (Al) O	485.5(23.7%)	486.2(58.4%)	487.0(17.9%)

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