尿素均匀沉淀法合成CeO2-Al2O3载体负载Pt催化剂的CO氧化性能

doi:10.11949/0438-1157.20250252

化工学报 ›› 2025, Vol. 76 ›› Issue (10): 5114-5127.DOI: 10.11949/0438-1157.20250252

• 催化、动力学与反应器 • 上一篇下一篇

尿素均匀沉淀法合成CeO₂-Al₂O₃载体负载Pt催化剂的CO氧化性能

杜宇鹏¹(), 葛春亮², 丁垒琳¹, 张力², 胡家俊¹, 俞峰苹², 林益¹, 王峰¹, 蒋师¹, 郭燏¹()

^1.南京工业大学化工学院材料化学工程全国重点实验室，江苏南京 211816
^2.浙江浙能科技环保集团股份有限公司，浙江杭州 310003

收稿日期:2025-03-14 修回日期:2025-06-05 出版日期:2025-10-25 发布日期:2025-11-25
通讯作者: 郭燏
作者简介:杜宇鹏（2000—），男，硕士研究生，202261104180@njtech.edu.cn
基金资助:
浙江省能源集团有限公司科学技术项目(ZNKJ-2024-076);国家自然科学基金项目(22108116);材料化学工程全国重点实验室自主课题项目(SKL-MCE-24A13)

CO oxidation performance of Pt catalysts supported on CeO₂-Al₂O₃ supports synthesized via urea homogeneous precipitation

Yupeng DU¹(), Chunliang GE², Leilin DING¹, Li ZHANG², Jiajun HU¹, Fengping YU², Yi LIN¹, Feng WANG¹, Shi JIANG¹, Yu GUO¹()

^1.State key Laboratory of Materials-oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, Jiangsu, China
^2.Zhejiang Zheneng Technology and Environment Group Co. , Ltd. , Hangzhou 310003, Zhejiang, China

Received:2025-03-14 Revised:2025-06-05 Online:2025-10-25 Published:2025-11-25
Contact: Yu GUO

摘要/Abstract

摘要：

选取氨水、碳酸铵、碳酸氢铵和尿素为沉淀剂，以高比表面积Al₂O₃作为非溶解性铝源，Ce(NO₃)₃·6H₂O作为可溶性铈源，通过沉积沉淀法合成CeO₂-Al₂O₃载体，经Pt浸渍负载制备了Pt/CeO₂-Al₂O₃催化剂，考察了沉淀剂类型对CO催化氧化性能的影响。表征结果表明，尿素均匀沉淀法制备的催化剂展现出最优活性，被归因于增强的Pt-CeO₂界面相互作用。沉淀剂类型通过调控结晶动力学和前体种类，影响了CeO₂的分散度、分布均匀性、形貌特征及其与Pt的相互作用。在Al₂O₃存在的尿素均匀沉淀中，限制孔道内的缓慢沉淀机制促进了纳米棒状CeO₂粒子在Al₂O₃孔道内的均匀分布且高度分散，避免了氨水沉淀剂因快速沉淀而引起的纳米球状CeO₂在Al₂O₃外表面上的富集团聚，从而强化了Pt与CeO₂间的相互作用，最终实现催化性能的提升。

关键词: 氧化铈, 氧化铝, 均匀沉淀, 铂, 一氧化碳, 催化

Abstract:

Four precipitating agents (ammonium hydroxide, ammonium carbonate, ammonium bicarbonate, and urea) were selected to synthesize CeO₂-Al₂O₃ supports via a precipitation method, using high-surface-area Al₂O₃ as a non-soluble aluminum source and Ce(NO₃)₃·6H₂O as a cerium precursor. Pt/CeO₂-Al₂O₃ catalysts were subsequently prepared by Pt impregnation to investigate the effect of precipitating agents on CO catalytic oxidation performance. Characterization results show that the catalyst prepared by urea uniform precipitation method exhibits the best activity, which is attributed to the enhanced Pt-CeO₂ interface interaction. The type of precipitant affects the dispersion, distribution uniformity, morphology of CeO₂, and the interaction between Pt and CeO₂ by altering crystallization kinetics and precursor types. In the urea homogeneous precipitation process with the presence of Al₂O₃, the slow precipitation mechanism within confined channels promotes both uniform distribution and high dispersion of nanorod-like CeO₂ particles inside the Al₂O₃ pores. This approach avoids the aggregation and surface enrichment of spherical CeO₂ nanoparticles on the outer surface of Al₂O₃ caused by rapid precipitation when using ammonia as a precipitant. Thereby, it strengthens the interaction between Pt and CeO₂, ultimately achieving enhanced catalytic performance.

Key words: cerium dioxide, alumina, homogeneous precipitation, platinum, carbon monoxide, catalysis

中图分类号:

TQ 426.8

杜宇鹏, 葛春亮, 丁垒琳, 张力, 胡家俊, 俞峰苹, 林益, 王峰, 蒋师, 郭燏. 尿素均匀沉淀法合成CeO₂-Al₂O₃载体负载Pt催化剂的CO氧化性能[J]. 化工学报, 2025, 76(10): 5114-5127.

Yupeng DU, Chunliang GE, Leilin DING, Li ZHANG, Jiajun HU, Fengping YU, Yi LIN, Feng WANG, Shi JIANG, Yu GUO. CO oxidation performance of Pt catalysts supported on CeO₂-Al₂O₃ supports synthesized via urea homogeneous precipitation[J]. CIESC Journal, 2025, 76(10): 5114-5127.

图/表 13

图1 不同催化剂上的CO转化率

Fig.1 CO conversion obtained on different catalysts

图2 不同催化剂的XRD谱图

Fig.2 XRD patterns of different catalysts

表1 不同催化剂上的比表面积、孔容、孔径、CeO2晶粒尺寸、Pt分散度和T90

Table 1 Specific surface area， pore volume， pore size， CeO2 grain size， Pt dispersion， and T90 on different catalysts

Sample	Specific surface area/(m²/g)	Total pore volume/(cm³/g)	Average pore diameter/nm	CeO₂grain size^①/nm	Pt dispersion^②/%	T₉₀/℃
Pt/CeAl-PAH	133	0.463	14.0	5.6	29	165
Pt/CeAl-PAC	130	0.459	14.1	11.8	49	161
Pt/CeAl-PAB	133	0.461	13.9	13.0	63	159
Pt/CeAl-HPU	133	0.449	13.6	9.3	69	149
Pt/CeAl-I	112	0.425	15.2	8.9	57	162
Pt/Al-I	140	0.476	13.3	—	41	174
Al₂O₃	142	0.478	13.5	—	—	—

图3 不同催化剂的XPS谱图

Fig.3 XPS spectra of different catalysts

表2 不同催化剂上的表面Ce原子浓度、Pt0比例、Ce3+比例和Osur比例

Table 2 Surface Ce atomic concentration， Pt0 ratio， Ce3+ ratio， and Osur ratio on different catalysts

Sample	Ce atomic concentration/%	[Pt⁰/(Pt ^δ⁺+Pt⁰)]/%	[Ce³⁺/(Ce³⁺+Ce⁴⁺)]/%	[O_sur/(O_sur+O_lat)]/%
Pt/CeAl-PAH	7.8	20.7	13.6	36.4
Pt/CeAl-PAC	9.9	27.2	15.3	38.0
Pt/CeAl-PAB	8.6	21.6	14.5	38.2
Pt/CeAl-HPU	1.7	51.2	20.8	43.0
Pt/CeAl-I	4.0	18.7	15.3	38.3
Pt/Al-I	—	30.6	—	32.6

图4 不同催化剂的H2-TPR谱图

Fig.4 H2-TPR profiles of different catalysts

图5 不同催化剂上T90(a)、Pt分散度(b)、Ce3+比例(c)、Osur比例(d)、H2-TPR的LTRP (e)及Pt 4f结合能偏移量(f)之间的关系

Fig.5 Relationships between T90 (a), Pt dispersion (b), Ce3+ ratio (c), Osur ratio (d), low-temperature peak temperature of H₂-TPR (e), and binding energy shift of Pt 4f (f) on different catalysts

图6 尿素均匀沉淀过程中pH随时间的变化

Fig.6 Variation of pH with time during the urea homogeneous precipitation process

图7 Ce3+(a)、Al2O3(b)和尿素(c)的含量对尿素均匀沉淀过程中pH经时变化趋势的影响

Fig.7 Effects of contents of Ce3+(a), Al2O3(b), and urea(c) on the time-dependent pH variation trend during the urea homogeneous precipitation

图8 不同沉淀法制得样品的XRD谱图

Fig.8 XRD patterns of samples prepared by different precipitation methods

图9 Ce-HPU-AD和CeAl-HPU-AD样品的热重分析

Fig.9 Thermogravimetric analysis of Ce-HPU-AD and CeAl-HPU-AD samples

图10 不同样品的TEM图和表面元素分布

Fig.10 TEM images and surface elemental distribution of different samples

表3 均匀沉淀过程中尿素含量对CeO2晶粒尺寸、比表面积、Pt分散度、H2-TPR的LTRP及T90的影响

Table 3 Effect of urea content in the homogeneous precipitation process on the grain size of CeO2， specific surface area， Pt dispersion， LTRP in H2-TPR， and T90

Sample	Ce³⁺/Al₂O₃/urea	CeO₂ grain size/nm	Specific surface area/(m²/g)	Pt dispersion	LTRP of H₂-TPR/℃	CO T₉₀/℃
Pt/CeAl-HPU₅	0.1/1.1/0.5	9.3	132	0.69	87	149
Pt/CeAl-HPU₁₅	0.1/1.1/1.5	11.4	137	0.61	97	154
Pt/CeAl-HPU₂₅	0.1/1.1/2.5	13.7	135	0.51	112	160

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尿素均匀沉淀法合成CeO₂-Al₂O₃载体负载Pt催化剂的CO氧化性能

CO oxidation performance of Pt catalysts supported on CeO₂-Al₂O₃ supports synthesized via urea homogeneous precipitation

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