Effects of Sm addition on reactivity and thermal stability of Pt/SBA-15 for catalytic complete oxidation of benzene

doi:10.11949/0438-1157.20191258

Abstract

Abstract:

The Sm addition effects on the reactivity and thermal stability of Pt/SBA-15 for catalytic complete oxidation of benzene were investigated. A simple method for recording the burning-off curves and the evaluation for the thermal stability of catalysts was adopted, that is, a constant flow of reaction gas was continuously introduced into a fixed bed reactor loaded with catalyst. The reaction temperature was increased step by step, and the on-line outlet concentrations of benzene were detected after time interval sampling. The burning-off curves could be recorded during this stage. After that, the reaction temperature was increased continuously, and kept at a certain value (e.g. 550℃), the on-line sampling analysis was kept at a set time. If necessary, the reaction temperature could be decreased step by step to check the activity variation of the catalyst. The results indicated that the activity order for four catalysts at lower temperature stage was Pt/SBA-15≈Pt/4%Sm₂O₃/SBA-15> Pt/Sm₂O₃> 4%Sm₂O₃/SBA-15, while the stability order at high temperature was Pt/4%Sm₂O₃/SBA-15> Pt/1.2%Sm₂O₃/SBA-15> Pt/SBA-15，Pt/Sm-SBA-15(SG)> Pt/SBA-15(SG). In conclusion, Sm can not improve the catalytic activity of Pt / SBA-15 at low temperature, but can significantly improve the stability of the catalyst at high temperature. At the same time, 1% Pt/4% Sm₂O₃ / SBA-15 has good catalytic activity at low temperature and high temperature stability, and has a good application prospect.

Key words: Sm₂O₃, Pt/SBA-15, benzene, catalysis, complete oxidation, thermal stability

摘要：

以Pt/SBA-15为催化剂，考察催化剂载体中添加Sm对于苯的完全氧化反应活性和热稳定性影响。采用了一种简便的记录起燃温度曲线和催化剂热稳定性评价方法，即向装载好催化剂的固定床反应器中持续通入恒定流量的反应气，逐步阶段性升高反应温度，同时在线检测出口尾气的浓度变化, 得到起燃温度曲线后，继续提高反应温度，然后恒定在某一设定的温度(如550℃)持续运行较长时间, 期间定时在线取样分析，如果有必要还可以连续考察降温情况下催化剂的反应活性情况。研究结果表明，几种催化剂低温活性次序为：Pt/SBA-15≈Pt/4%Sm₂O₃/SBA-15> Pt/Sm₂O₃> 4%Sm₂O₃/SBA-15,而对于高温稳定性则是Pt/4%Sm₂O₃/SBA-15> Pt/1.2%Sm₂O₃/SBA-15> Pt/SBA-15，Pt/Sm-SBA-15(SG)> Pt/SBA-15(SG)。总之，Sm的添加虽然未能提高Pt/SBA-15的低温催化活性，但是能明显提高催化剂在高温情况下活性的稳定性。1%Pt/4%Sm₂O₃/SBA-15同时具备较好的低温催化活性和高温稳定性，具有较好的应用前景。

关键词: Sm₂O₃, Pt/SBA-15, 苯, 催化, 完全氧化, 热稳定性

CLC Number:

TQ 426

Jianxin MAO, Ziqing YUAN, Hongxiao YANG, Renxian ZHOU. Effects of Sm addition on reactivity and thermal stability of Pt/SBA-15 for catalytic complete oxidation of benzene[J]. CIESC Journal, 2020, 71(1): 306-313.

毛建新, 袁子卿, 严红绡, 周仁贤. 添加Sm对Pt /SBA-15催化苯完全氧化反应活性和热稳定性的影响[J]. 化工学报, 2020, 71(1): 306-313.

Figures/Tables 9

Table 1 Pore diameter, SBET and pore volume of some catalysts

No.	Catalyst	Pt/ %(mass)	Sm₂O₃/ %(mass)	Pore diameter/ nm	S_BET/ (m²/g)	V_pore/ (cm³/g)
1	SBA-15	0	0	10.6	473	1.22
2	Pt/SBA-15	1	0	8.0	355	0.84
3	Pt/1.2%Sm₂O₃/SBA-15	1	1.2	9.0	455	1.01
4	Pt/4%Sm₂O₃/SBA-15	1	4.0	7.9	442	1.08
5	Pt/SBA-15(SG)	1	0	5.2	428	0.71
6	Pt/Sm-SBA-15(SG)	1	4.0	3.6	371	0.43

Fig.1 Adsorption and desorption isotherm and pore volume distribution of Pt/Sm-SBA-15(SG) sample

Fig.2 XRD patterns of three catalysts before and after reaction

Fig.3 HAADF-STEM image of 1%Pt/SBA-15 and column distribution graph of Pt particle diameter

Fig.4 HAADF-STEM image of 1%Pt/4%Sm2O3/SBA-15 as well as corresponding element O, Si, Sm and Pt maps

Fig.5 Relationship of complete oxidation conversion of benzene with reaction temperature over several catalysts

Fig.6 Relationship of benzene conversion with reaction time at higher temperature over 1%Pt/SBA-15 and Sm2O3/SBA-15 respectively

Fig.7 Relationship of conversion of benzene with reaction time at higher temperature over 1%Pt/4% Sm2O3/SBA-15 and 1%Pt/1.2% Sm2O3/SBA-15 respectively

Fig.8 Reaction stability comparison of 1%Pt/SBA-15(SG) and 1%Pt/Sm-SBA-15(SG) at higher temperature

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