不同碱辅助的沉积沉淀法对三效催化剂稳定性的影响

doi:10.15541/jim20200357

无机材料学报 ›› 2021, Vol. 36 ›› Issue (6): 659-664.DOI: 10.15541/jim20200357

不同碱辅助的沉积沉淀法对三效催化剂稳定性的影响

范君¹(), 江雪², 焦毅²(), 陈宇圣¹, 王健礼¹(), 陈耀强¹^,²

1.四川大学化学学院, 成都 610064
2.四川大学新能源与低碳技术研究院, 成都 610064

收稿日期:2020-06-29 修回日期:2020-09-17 出版日期:2021-06-20 网络出版日期:2020-10-10
通讯作者: 焦毅, 教授. E-mail: jiaoyiscu@163.com; 王健礼, 教授. E-mail: wangjianli@scu.edu.cn
作者简介:范君(1996-), 女, 硕士研究生. E-mail: fj960117@163.com

Effect of Different Alkali-assisted Deposition Precipitation Methods on the Durability of Three-way Catalysts

FAN Jun¹(), JIANG Xue², JIAO Yi²(), CHEN Yusheng¹, WANG Jianli¹(), CHEN Yaoqiang¹^,²

1. College of Chemistry, Sichuan University, Chengdu 610064, China
2. Institute of New Energy and Low-Carbon Technology, Sichuan University, Chengdu 610064, China

Received:2020-06-29 Revised:2020-09-17 Published:2021-06-20 Online:2020-10-10
Contact: JIAO Yi, professor. E-mail: jiaoyiscu@163.com; WANG Jianli, professor. E-mail: wangjianli@scu.edu.cn
About author:FAN Jun (1996-), female, Master candidate. E-mail: fj960117@163.com
Supported by:
National Natural Sciece Foundation of China(22072097);Sichuan Science and Technology Program(2019YFS0498)

摘要/Abstract

摘要：

老化处理会导致三效催化剂(TWCs)严重失活, 因此提高催化剂的耐久性能是TWCs设计的目标。本工作采用不同碱辅助的沉积沉淀法, 即尿素辅助沉积沉淀法和氨水辅助沉积沉淀法制备了Pt/Ce_0.4Zr_0.5La_0.05Pr_0.05O₂ (Pt/CZ)三效催化剂, 分析了不同碱对催化剂物理化学性质、催化活性和耐久性的影响。结果表明, 尿素辅助沉积沉淀法(UDP)制备的Pt/CZ催化剂的抗老化性能较差, 而氨水辅助沉积沉淀法(ADP)制备的催化剂的抗老化能力较强。XRD, CO 吸附, XPS和H₂-TPR表征结果表明, ADP中较大的Pt颗粒以及更强的金属载体相互作用使ADP在老化过程中烧结程度较低, 有利于维持催化活性。因此, ADP催化剂具有一定的工业应用前景。

关键词: 三效催化剂, 沉积沉淀, 碱辅助, 稳定性

Abstract:

The aging treatment always brings about severe deactivation of three-way catalysts (TWCs) so that improving the durability is one goal of TWCs design. In this work, Pt/Ce_0.4Zr_0.5La_0.05Pr_0.05O₂ (Pt/CZ) TWCs were prepared by two different alkali-assisted deposition precipitation method, urea or ammonia. The effects of different alkali-assisted on the physicochemical properties, catalytic activity and durability were analyzed. It was found that the Pt/CZ catalyst prepared by urea-assisted deposition precipitation method (UDP) had poor aging resistance but the Pt/CZ catalyst prepared by ammonia-assisted (ADP) showed better anti-aging ability. Based on the results of XRD, CO adsorption, XPS and H₂-TPR, comparatively larger particle size of Pt species and stronger interaction for ADP make it more difficult to sinter together during the aging treatment, which is favorable for maintaining catalytic activity. Therefore, the ADP catalyst shows a bright future for industrialization.

Key words: three-way catalysts, deposition precipitation, alkali-assisted, durability

中图分类号:

O643

范君, 江雪, 焦毅, 陈宇圣, 王健礼, 陈耀强. 不同碱辅助的沉积沉淀法对三效催化剂稳定性的影响[J]. 无机材料学报, 2021, 36(6): 659-664.

FAN Jun, JIANG Xue, JIAO Yi, CHEN Yusheng, WANG Jianli, CHEN Yaoqiang. Effect of Different Alkali-assisted Deposition Precipitation Methods on the Durability of Three-way Catalysts[J]. Journal of Inorganic Materials, 2021, 36(6): 659-664.

图/表 8

Table 1 Textural and structural parameters of the support and samples

Samples	Surface area/ (m²•g^-1)	Pore volume/ (mL•g^-1)	Average pore radius/nm
IM	60	0.23	7.5
UDP	63	0.22	7.5
ADP	61	0.23	7.7
IM-a	49	0.24	9.4
UDP-a	50	0.22	7.6
ADP-a	53	0.25	7.7
CZLP	64	0.25	8.7

Fig. 1 XRD patterns of fresh and aged samples (a) and the comparison of their relative intensities of Pt (111) based on the strongest peak of support (b)

Fig. 2 Pt dispersion of samples measured by CO-chemisorption method (a) and FT-IR spectra of CO absorbed on the fresh (b) and aged (c) samples

Fig. 3 XPS spectra of O1s (a, d), Ce3d (b, e) and Pt4f (c, f) for fresh (a-c) and aged (d-f) samples

Table 2 Surface elemental state ratio derived from by XPS

Sample	Pt⁰/Pt ratio	Pt²⁺/Pt ratio	Pt⁴⁺/Pt ratio	O_ads/O ratio	Ce³⁺/Ce ratio
IM	0	0.871	0.129	0.354	0.217
UDP	0	0.851	0.149	0.374	0.240
ADP	0	0.831	0.169	0.324	0.201
IM-a	0.302	0.698	0	0.329	0.195
UDP-a	0.421	0.579	0	0.350	0.187
ADP-a	0.234	0.766	0	0.336	0.214

Fig. 4 H2-TPR profiles of the fresh (a) and aged (b) samples

Fig. 5 Conversion curves of CO, NO, C3H8 and C3H6 over the fresh (a-d) and aged (e-h) samples, respectively

Table 3 Light-off (T50) temperature and ΔT for three-way catalytic reactions over catalysts

Sample	CO		NO		C₃H₈		C₃H₆
Sample	T₅₀/℃	ΔT /℃	T₅₀/℃	ΔT/℃	T₅₀/℃	ΔT/℃	T₅₀/℃	ΔT/℃
IM	174	-	260	-	269	-	234	-
UDP	142	-	259	-	273	-	228	-
ADP	187	-	277	-	284	-	254	-
IM-a	215	41	304	44	312	43	278	44
UDP-a	229	87	313	54	328	55	287	59
ADP-a	203	16	294	17	306	22	272	18

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不同碱辅助的沉积沉淀法对三效催化剂稳定性的影响

Effect of Different Alkali-assisted Deposition Precipitation Methods on the Durability of Three-way Catalysts

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