自发氧化还原法制备Co3O4/CeO2纳米复合材料及其CO催化氧化反应结构优化

doi:10.7503/cjcu20190649

高等学校化学学报 ›› 2020, Vol. 41 ›› Issue (4): 652.doi: 10.7503/cjcu20190649

• 庆祝《高等学校化学学报》复刊40周年专栏 • 上一篇下一篇

自发氧化还原法制备Co₃O₄/CeO₂纳米复合材料及其CO催化氧化反应结构优化

金欣¹,冯锡岚¹,刘大鹏^1,^*(),苏雨童¹,张政¹,张瑜^1,^2,^3,^*()

^1. 北京航空航天大学化学学院, 仿生智能界面科学与技术教育部重点实验室
^2. 国际交叉科学研究院
^3. 生物医学工程高级创新中心, 北京100191

收稿日期:2019-12-11 出版日期:2020-04-10 发布日期:2020-02-17
通讯作者: 刘大鹏,张瑜 E-mail:liudp@buaa.edu.cn;jade@buaa.edu.cn
基金资助:
国家自然科学基金(51972008, 51925202)

Auto-redox Strategy for the Synthesis of Co₃O₄/CeO₂ Nanocomposites and Their Structural Optimization Towards Catalytic CO Oxidation

JIN Xin¹,FENG Xilan¹,LIU Dapeng^1,^*(),SU Yutong¹,ZHANG Zheng¹,ZHANG Yu^1,^2,^3,^*()

^1. Key Laboratory of Bio?inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry
^2. International Research Institute for Multidisciplinary Science
^3. Beijing Advanced Innovation Center for Biomedical Engineering, Beihang University, Beijing 100191, China

Received:2019-12-11 Online:2020-04-10 Published:2020-02-17
Contact: Dapeng LIU,Yu ZHANG E-mail:liudp@buaa.edu.cn;jade@buaa.edu.cn
Supported by:
This paper is supported by the National Natural Science Foundation of China(51972008, 51925202)

摘要/Abstract

关键词: 四氧化三钴, 二氧化铈, 自发氧化还原法, 一氧化碳氧化

Abstract:

A simple auto-redox strategy was successfully used to synthesize Co₃O₄/CeO₂ nanocomposites. These samples were then characterized by means of TEM, XRD, XPS, and so on, to study the influence of reaction parameters on their catalyst activity. The results indicate that the catalytic performance of Co₃O₄/CeO₂ nanocomposites could be optimized by changing the molar ratio of Co/Ce, pH values, reaction and calcination temperatures. The optimal Co₃O₄/CeO₂ nanocomposite could reach a 100% CO conversion at 140 ℃ compared to the others. Moreover its catalytic activity kept stable after cycling, indicating its good stability.

Key words: Co₃O₄, CeO₂, Auto-redox, CO oxidation

中图分类号:

O643

TrendMD:

金欣, 冯锡岚, 刘大鹏, 苏雨童, 张政, 张瑜. 自发氧化还原法制备Co₃O₄/CeO₂纳米复合材料及其CO催化氧化反应结构优化. 高等学校化学学报, 2020, 41(4): 652.

JIN Xin, FENG Xilan, LIU Dapeng, SU Yutong, ZHANG Zheng, ZHANG Yu. Auto-redox Strategy for the Synthesis of Co₃O₄/CeO₂ Nanocomposites and Their Structural Optimization Towards Catalytic CO Oxidation. Chem. J. Chinese Universities, 2020, 41(4): 652.

图/表 12

Scheme 1 Synthetic process of Co3O4/CeO2 nanocomposites

Fig.1 TEM images(A—H) and XRD patterns(I, J) of Co3O4/CeO2 samples before(A—D, I) and after calcination(E—H, J)(A, E) Co1/Ce5; (B, F) Co5/Ce1; (C, G) Co9/Ce1; (D, H) Co15/Ce1; (I, J) a. CeO2; b. Co1/Ce5; c. Co5/Ce1; d. Co9/Ce1; e. Co15/Ce1.

Fig.2 CO conversions of Co3O4/CeO2 samples with different molar ratios of Co/Ce

Fig.3 CO conversions of Co3O4/CeO2 samples with different amounts of NaOH(aq)

Fig.4 CO conversions of Co3O4/CeO2 samples prepared at different temperatures

Fig.5 CO conversions of Co9/Co1-tC-300, Co9/Co1-tC-400 and Co9/Co1-tC-500

Fig.6 TEM(A), HRTEM(B) images and mapping analysis(C—F) of Co9/Ce1-tC-400

Fig.7 XPS spectra of Ce3d(A), Co2p(B), O1s(C) of Co9/Ce1-tC-400

Table 1 BET surface area, pore volumes and pore sizes of pure Co3O4, CeO2 and Co9/Ce1 samples calcinated at 300, 400 and 500 ℃

Sample	S_BET/(m²·g^-1)	Pore volume/(cm³·g^-1)	Pore size/nm
Co₉/Ce₁-t_C-300	113.6700	0.230290	6.3285
Co₉/Ce₁-t_C-400	95.2122	0.277253	9.4890
Co₉/Ce₁-t_C-500	77.2589	0.221758	9.2293
Co₃O₄	19.5577	0.189476	29.7476
CeO₂	74.7081	0.097905	3.9790

Fig.8 H2-TPR profiles of Co9/Ce1(a), Co9/Ce1-3NaOH(b), Co9/Ce1-tR-60(c), Co9/Ce1-tC-400(d), Co3O4(e) and CeO2(f)

Fig.9 Cycling test curves of Co3O4/CeO2 nanocomposites

Table 2 Catalytic activity for CO oxidation of Co3O4/CeO2 composites reported in the literatures

Sample	Amount of catalyst/mg	Feed gas	t₁₀₀/℃	Ref.
Co₃O₄@CeO₂ core@shell cubes	25	1%CO/20%O₂/79%N₂(30 mL/min)	190	[18]
CeO₂/Co₃O₄ yolk-shell nanospheres	100	1%CO/99%Air(30 mL/min)	110	[28]
Co₃O₄/CeO₂ nanosheets	30	1%CO/99%Air(30 mL/min)	140	[29]
CeO₂/Co₃O₄ nanojunctions	50	1%CO/99%Air(30 mL/min)	110	[32]
CeO₂@Co₃O₄ core@shell microspheres	50	1%CO/20%O₂/79%N₂(50 mL/min)	170	[31]
Co₃O₄/CeO₂ composites	25	1%CO/99%Air(30 mL/min)	140	This work

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自发氧化还原法制备Co₃O₄/CeO₂纳米复合材料及其CO催化氧化反应结构优化

Auto-redox Strategy for the Synthesis of Co₃O₄/CeO₂ Nanocomposites and Their Structural Optimization Towards Catalytic CO Oxidation

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