CuO-CeO2/TiO 2 高效催化CO低温氧化反应性能

doi:10.16085/j.issn.1000-6613.2022-1832

摘要/Abstract

摘要：

利用等体积浸渍法制备了CuO-CeO₂/TiO₂催化剂，用于低温CO氧化反应。考察了焙烧温度、Cu-Ce负载量和Ce/Cu摩尔比等对CuO-CeO₂/TiO₂催化性能的影响，利用XRD、N₂等温吸附-脱附、XPS、H₂-TPR等方法对催化剂进行了表征。结果表明，当n_Ce/n_Cu为1.6，Cu-Ce负载量为30%时，经500℃焙烧所制得催化剂具有最佳催化活性；当空速为24000mL/（g·h），在该催化剂上90℃时CO可完全氧化。表征发现，CuO-CeO₂/TiO₂催化剂表面较高的Ce³⁺、Cu⁺和吸附氧含量有利于催化CO氧化反应。制备条件通过影响催化剂表面的Ce³⁺、Cu⁺和吸附氧含量，影响催化剂活性。其中，焙烧温度、Cu-Ce负载量和n_Ce/n_Cu均会影响CuO-CeO₂/TiO₂表面Cu⁺和吸附氧含量，而催化剂表面Ce³⁺含量仅受Cu-Ce负载量的影响较大。

关键词: 一氧化碳, 氧化, 催化剂, 制备条件

Abstract:

CuO-CeO₂/TiO₂ catalyst was prepared by incipient impregnation method and then used for CO oxidation at low temperature. The effects of calcination temperature, Cu-Ce loading and Ce/Cu molar ratio on the catalytic performance of CuO-CeO₂/TiO₂ were investigated. The catalyst was characterized by XRD, N₂ isothermal adsorption-desorption, XPS and H₂-TPR. When n_Ce/n_Cu was 1.6, and Cu-Ce loading was 30%, the catalyst calcined at 500℃ showed the best catalytic activity. When GHSV was 24000mL/(g·h), CO can be completely oxidized on the catalyst at 90℃. It was found that the high content of Ce³⁺, Cu⁺ and adsorbed oxygen on the surface of CuO-CeO₂ /TiO₂ catalyst was favorable to catalyze CO oxidation. The preparation conditions could affect the catalyst activity by regulating the content of Ce³⁺, Cu⁺ and adsorbed oxygen on the catalyst surface. Among them, calcination temperature, Cu-Ce loading and n_Ce/n_Cu would influence the contents of Cu⁺ and adsorbed oxygen on CuO-CeO₂/TiO₂ surface, while Cu-Ce loading has greatly impact on the Ce³⁺ content on catalyst surface.

Key words: carbon monoxide, oxidation, catalyst, preparation conditions

中图分类号:

O643

李润蕾, 王子彦, 王志苗, 李芳, 薛伟, 赵新强, 王延吉. CuO-CeO₂/TiO ₂ 高效催化CO低温氧化反应性能[J]. 化工进展, 2023, 42(8): 4264-4274.

LI Runlei, WANG Ziyan, WANG Zhimiao, LI Fang, XUE Wei, ZHAO Xinqiang, WANG Yanji. Efficient catalytic performance of CuO-CeO₂/TiO₂ for CO oxidation at low-temperature[J]. Chemical Industry and Engineering Progress, 2023, 42(8): 4264-4274.

图/表 17

参考文献 55

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编号	催化剂参数	数值
编号	催化剂参数	10%	20%	30%	40%
1	CeO₂晶粒尺寸/nm	4.8	5.4	6.8	7.0
2	CeO₂晶格常数/nm	0.5406	0.5400	0.5381	0.5389
3	S_BET/m²·g^-1	52.2	52.5	55.6	54.1
4	平均孔容/cm³·g^-1	0.26	0.21	0.20	0.18
5	平均孔径/nm	15.5	14.4	11.0	10.4
6	[Ce³⁺/（Ce³⁺+Ce⁴⁺）]/%	15.7	17.7	18.9	14.9
7	（I_sat/I_pp）/%	30.4	29.3	27.6	29.0
8	[O_ads/（O_ads+O_latt）]/%	15.1	17.4	26.6	19.6

编号	催化剂参数	数值
编号	催化剂参数	10%	20%	30%	40%
1	CeO₂晶粒尺寸/nm	4.8	5.4	6.8	7.0
2	CeO₂晶格常数/nm	0.5406	0.5400	0.5381	0.5389
3	S_BET/m²·g^-1	52.2	52.5	55.6	54.1
4	平均孔容/cm³·g^-1	0.26	0.21	0.20	0.18
5	平均孔径/nm	15.5	14.4	11.0	10.4
6	[Ce³⁺/（Ce³⁺+Ce⁴⁺）]/%	15.7	17.7	18.9	14.9
7	（I_sat/I_pp）/%	30.4	29.3	27.6	29.0
8	[O_ads/（O_ads+O_latt）]/%	15.1	17.4	26.6	19.6

编号	催化剂参数	数值
编号	催化剂参数	300℃	400℃	500℃	600℃
1	CeO₂晶粒尺寸/nm	6.7	7.2	6.8	9.1
2	CeO₂晶格常数/nm	0.5399	0.5398	0.5381	0.5376
3	S_BET/m²·g^-1	75.5	69.8	55.6	34.0
4	平均孔容/cm³·g^-1	0.20	0.20	0.20	0.19
5	平均孔径/nm	9.2	9.0	11.0	17.8
6	[Ce³⁺/（Ce³⁺+Ce⁴⁺）]/%	19.4	18.7	18.9	18.6
7	（I_sat/I_pp）/%	29.1	30.1	27.6	29.5
8	[O_ads/（O_ads+O_latt）]/%	21.0	21.9	26.6	19.8

编号	催化剂参数	数值
编号	催化剂参数	300℃	400℃	500℃	600℃
1	CeO₂晶粒尺寸/nm	6.7	7.2	6.8	9.1
2	CeO₂晶格常数/nm	0.5399	0.5398	0.5381	0.5376
3	S_BET/m²·g^-1	75.5	69.8	55.6	34.0
4	平均孔容/cm³·g^-1	0.20	0.20	0.20	0.19
5	平均孔径/nm	9.2	9.0	11.0	17.8
6	[Ce³⁺/（Ce³⁺+Ce⁴⁺）]/%	19.4	18.7	18.9	18.6
7	（I_sat/I_pp）/%	29.1	30.1	27.6	29.5
8	[O_ads/（O_ads+O_latt）]/%	21.0	21.9	26.6	19.8

编号	催化剂参数	数值
编号	催化剂参数	n_Ce/n_Cu=1.2	n_Ce/n_Cu=1.4	n_Ce/n_Cu=1.6	n_Ce/n_Cu=1.8
1	CeO₂晶粒尺寸/nm	5.9	6.3	6.8	6.7
2	CeO₂晶格常数/nm	0.5389	0.5387	0.5381	0.5382
3	S_BET/m²·g^-1	45.4	55.4	55.6	54.2
4	平均孔容/cm³·g^-1	0.17	0.19	0.20	0.20
5	平均孔径/nm	13.8	10.9	11.0	10.8
6	[Ce³⁺/（Ce³⁺+Ce⁴⁺）]/%	17.0	17.6	18.9	17.9
7	（I_sat/I_pp）/%	30.6	27.9	27.6	29.5
8	[O_ads/（O_ads+O_latt）]/%	21.9	19.2	26.6	18.6

CuO-CeO₂/TiO ₂ 高效催化CO低温氧化反应性能

Efficient catalytic performance of CuO-CeO₂/TiO₂ for CO oxidation at low-temperature

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参考文献 55

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催化剂	原料气组成及体积分数	空速/mL·g^-1·h^-1	T/℃	CO转化率/%	参考文献
CuO-CeO₂/TiO₂	1% CO, 9% O₂, N₂	24000	90	100	本文
Pt/Cr_1.3Fe_0.7O₃	1% CO, 1% O₂, N₂	120000	80	78.8	[43]
Ag/CeO₂	0.2% CO, 1% O₂, N₂	240000	230	50	[44]
Au-CeO₂	0.05%~1% CO, 10%O₂, He	2650	25	100	[6]
Mn₃O₄/CeO₂	1%CO, 4% O₂, He	60000	194	90	[45]
CuO-CeO₂/UiO-66	1% CO, 3% O₂, N₂	24000	160	99	[46]
Co₃O₄ NAs-6	1% CO, 20% O₂, N₂	10000h^-1	150	100	[47]
NiO/CeO₂	0.6% CO, 1.5% O₂, Ar	60000	200	99.2	[48]
CuO-CeO₂/C	1% CO, 21% O₂, He	45000h^-1	150	100	[49]
Au-CeO₂/SiO₂	1% CO, 干空气	12000	210	100	[50]
Cu_aCe_bFe_c-PSF	180mL/m³ CO, 空气	7643h^-1	200	100	[51]
Cu₁/MnO₂	1% CO, 15% O₂, He	34000	80	90	[52]
CoMn-a	2% CO, 20% O₂, Ar	60000	125	100	[53]
NiO-CuO	2% CO, 5% O₂, Ar	60000	138	100	[54]
CuO/CeO₂-20	0.4% CO, 空气	8000	110	100	[55]

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