介孔片状NiO/Co<sub>3</sub>O<sub>4</sub>催化剂催化碳烟燃烧性能研究

孙红华; 孙彪; 李鹏; 邱健强; 张念陈; 王金果; 王秀通

doi:10.12299/jsues.22-0064

介孔片状NiO/Co₃O₄催化剂催化碳烟燃烧性能研究

doi: 10.12299/jsues.22-0064

1.
上海工程技术大学化学化工学院, 上海 201620
2.
中国科学院海洋研究所, 青岛 266071

基金项目: 国家自然科学基金面上项目资助（22076117）；上海市自然科学基金项目资助（20ZR1422500）；上海市松江区第五届拔尖人才培养资助计划

详细信息

作者简介:
孙红华（1994−），男，硕士，研究方向为柴油车尾气净化. E-mail：18605625362@163.com

通讯作者:
王金果（1982−），男，教授，博士，研究方向为环境污染控制. E-mail：Jinguowang1982@sues.edu.cn

中图分类号: O643.32
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- 被引次数: 0
出版历程
- 收稿日期: 2022-03-22
- 刊出日期: 2023-06-20

Research on Enhanced catalytic soot combustion performance over NiO/Co₃O₄ within mesoporous nanosheets

1.
School of Chemistry and Chemical Engineering, Shanghai University of Engineering Science, Shanghai 201620, China
2.
Institute of Oceanology, Chinese Academy of Sciences, Qingdao 266071, China

摘要

摘要: 采用水热结合等体积浸渍法制备一系列NiO/Co₃O₄介孔纳米片催化剂，并以柴油机碳烟催化燃烧为模型反应评价其催化性能. 研究表明，当Ni/Co物质的量比为12%时，所制备的催化剂12NiCo具有最佳碳烟颗粒催化燃烧活性，其T_m为347 ℃，CO₂选择性为100%，主要归因于以下原因：1）二维片状结构及其较高的比表面积有效增大了催化剂与碳烟颗粒的接触界面；2）纳米片具有丰富的介孔孔道，有利于降低传质阻力，进而促进气体反应物的吸附与扩散；3）NiO的引入增强了催化剂的氧化还原能力，促进了氧物种的吸附与活化生成活性氧物种，同时也促进了NO氧化形成氧化能力更强的NO₂参与反应，进一步提升催化活性. 此外，该催化剂12NiCo具有良好的循环使用性能，显示了一定的潜在实用价值.
- 柴油机尾气 /
- 碳烟颗粒 /
- NiO/Co₃O₄ /
- 介孔纳米片 /
- 催化燃烧
Abstract: A series of NiO/Co₃O₄ catalysts within mesoporous nanosheets, synthesized by a facile hydrothermal combining wet-impregnation route, have been developed to catalyze diesel soot combustion. Results attest that, when the molar ratio of Ni/Co reached 12%, the catalyst of 12NiCo exhibited the optimal catalytic soot combustion performance, giving T_m of 347 ℃ and 100% CO₂ selectivity, which can be chiefly credited to the synergetic effect of the following factors. Firstly, the unique 2D nanosheets together with high surface area enlarged the contact interface of catalyst-soot particles. Secondly, abundant mesopores within nanosheets favored the significant decrease in mass transfer resistance and then in turn promoted the adsorption and diffusion of gas reactants. Thirdly, the enhanced reducibility by introducing NiO not merely facilitated the adsorption and activation of oxygen species to form active oxygen species, but also benefited NO oxidation to produce NO₂ with higher oxidative capability, thereby improving catalytic soot combustion performance remarkably. In addition, 12NiCo also presented the excellent reusability, demonstrating good potential in future practical applications.
- diesel exhaust /
- soot particles /
- NiO/Co₃O₄ /
- mesoporous nanosheets /
- catalytic combustion

HTML全文

图 1 不同催化剂的场发射扫描电镜图

Figure 1. FESEM images of different catalysts

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图 2 不同催化剂的XRD谱图

Figure 2. XRD patterns of different catalysts

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图 3 不同催化剂的拉曼光谱图

Figure 3. Raman spectra of different catalysts

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图 4 不同催化剂低温N₂吸脱附等温线和孔径分布曲线

Figure 4. N₂ adsorption-desorption isotherms and pore size distribution curves of different catalysts

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图 5 不同催化剂的XPS谱图

Figure 5. XPS spectra of different catalysts

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图 6 不同催化剂的H₂-TPR谱图

Figure 6. H₂-TPR profiles of different catalysts

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图 7 不同催化剂碳烟催化燃烧曲线图和柱状图

Figure 7. Activity date curve and histogram of soot combustion over different catalysts

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图 8 不同催化剂动力学测试图

Figure 8. Kinetic diagram of different catalysts

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图 9 催化剂12NiCo活性循环测试活性图及柱状图

Figure 9. Stability test and histogram of 12NiCo

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表 1 不同催化剂的物理结构参数及H₂消耗量

Table 1. Physicochemical parameters and H₂ consumption of different catalysts

Catalyst	S_BET/ (m²•g⁻¹)	V_P/ (cm³•g⁻¹)	D_P/ nm	Crystallize size/ nm	H₂ consumption/ (mmol•g⁻¹)
Co₃O₄	20	0.094	24	29.0	12.1
2NiCo	19	0.091	22	15.4	12.4
7NiCo	17	0.087	20	13.0	12.5
12NiCo	15	0.074	19	12.1	12.8
20NiCo	11	0.051	18	10.9	12.6
30NiCo	9	0.022	15	10.3	12.5

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表 2 不同催化剂的元素组成及价态参数

Table 2. Elemental composition and chemical valence states of different catalysts

Catalyst	Ni•2p			Co•2p			O•1s
Catalyst	Ni²⁺ /%	Ni³⁺ /%	Ni³⁺ /Ni²⁺	Co²⁺ /%	Co³⁺ /%	Co³⁺ /Co²⁺	O_{ads /}%	O_latt /%	O_ads /O_latt
Co₃O₄	—	—	—	48	52	1.08	25	75	0.33
2NiCo	51	49	0.96	47	53	1.13	40	60	0.67
7NiCo	60	40	0.67	45	55	1.22	49	51	0.96
12NiCo	67	33	0.49	42	58	1.38	63	37	1.70
20NiCo	55	45	0.81	46	54	1.17	84	16	5.25
30NiCo	52	48	0.92	50	50	1.00	90	10	9.0

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