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化学进展 2019, Vol. 31 Issue (6): 811-830 DOI: 10.7536/PC181042 前一篇   后一篇

• •

锰铈二元氧化物的制备与应用

刘德培, 田敬, 李静莎, 唐正, 王海燕**(), 唐有根**()   

  1. 中南大学化学化工学院 化学电源湖南省重点实验室 锰资源高效清洁利用湖南省重点实验室 长沙 410083
  • 收稿日期:2018-11-01 出版日期:2019-06-15 发布日期:2019-04-26
  • 通讯作者: 王海燕, 唐有根
  • 基金资助:
    国家自然科学基金项目(21571189); 国家自然科学基金项目(21671200); 湖南省科技计划项目(2017TP1001); 湖南省科技计划项目(2016TP1007); 中南大学创新驱动项目(2016CXS009)
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Preparation and Applications of Mn-Ce Binary Oxides

Depei Liu, Jing Tian, Jingsha Li, Zheng Tang, Haiyan Wang**(), Yougen Tang**()   

  1. Hunan Provincial Key Laboratory of Chemical Power Sources, Hunan Provincial Key Laboratory of Efficient and Clean Utilization of Manganese Resources,College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China
  • Received:2018-11-01 Online:2019-06-15 Published:2019-04-26
  • Contact: Haiyan Wang, Yougen Tang
  • About author:
    ** E-mail: (Haiyan Wang);
    (Yougen Tang)
  • Supported by:
    National Natural Science Foundation of China(21571189); National Natural Science Foundation of China(21671200); Hunan Provincial Science and Technology Plan Project, China(2017TP1001); Hunan Provincial Science and Technology Plan Project, China(2016TP1007); Innovation-Driven Project of Central South University(2016CXS009)

Mn-Ce二元氧化物具有资源丰富、成本低廉、催化活性优异等优点,引起了科研人员的广泛关注,在诸多领域具有潜在的应用价值。本文详细阐述了Mn-Ce二元氧化物的合成方法和应用领域。合成方法包括沉淀法、溶胶-凝胶法、水热法、浸渍法等,并比较了各方法的优缺点。在应用方面,主要综述了Mn-Ce二元氧化物在空气污染物消除(消除NOx、VOCs、CO、碳烟、Hg0、甲醛)和能源储存(金属-空气电池、超级电容器)两个方面的应用及其作用机制。另外,本文还介绍了Mn-Ce二元氧化物在水污染治理(氟离子吸附、三价砷吸附和甲基橙吸附等)和有机催化合成方面的应用。最后,讨论了Mn-Ce二元氧化物在制备中存在的问题,并对之后的研究方向进行了展望。

关键词： Mn-Ce二元氧化物, 合成方法, 污染治理, 能源存储, 有机催化

Mn-Ce binary oxide has been considered as a kind of outstanding materials and widely applied to many fields by the reasons of abundance, low cost, excellent oxygen storage and release capability and high catalytic performance. In this review, the preparation and applications of Mn-Ce binary oxides have been reviewed in detail. Preparation methods including precipitation method, sol-gel method, hydrothermal method, impregnation method, and so on, are summarized. Meanwhile, their merits and demerits are compared. As for applications, air pollution removal(NOx, VOCs, CO, soot, Hg0and formaldehyde) and energy storage systems(supercapacitors and metal-air batteries) are overviewed particularly. In addition, the applications of water pollution disposal(fluoride adsorbed, As(Ⅲ) removal, methyl orange degradation) and organic catalytic synthesis are introduced briefly. Finally, the main problems of preparation methods of Mn-Ce binary oxides are discussed and the research directions are forecast.

Key words: Mn-Ce binary oxides, synthesis methods, pollution disposal, energy storage, organic catalysis
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表1 锰氧化物的晶体结构
Table 1 Crystal structure of manganese oxides
Ingredient Crystal system Annotation
MnO Cubic Manganosite
α-Mn2O3 Rhombohedral
γ-Mn2O3 Cubic Bixbyite
Mn3O4 (Normal) Tetragonal Spinel structure
Mn3O4 (T ≥1443 K) Cubic Inverted spinel structure
α-MnO2 Tetragonal
β-MnO2 Tetragonal Pyrolusite
γ-MnO2 Hexagonal Hexagonal closest packed
λ-MnO2 Cubic Spinel
δ-MnO2 Hexagonal
Mn5O8 Monoclinic
图1 CeO2晶体结构
Fig. 1 Crystal structure of CeO2
图2 花状Mn掺杂CeO2的合成和SEM图[16]
Fig. 2 Schematic illustration of synthesis process and SEM image of flower like Mn-doped CeO2[16]
图3 (A)Mn-CeOx/CNTs的合成;(B,C)酸处理碳纳米管和Mn-CeOx/CNTs的TEM图[19]
Fig. 3 (A) Chematic illustration of synthesis process of Mn-CeOx/CNTs;(B, C) TEM images of acid-treated CNTs and Mn-CeOx/CNTs[19]
图4 溶胶-凝胶法制备Mn-Ce二元氧化物示意图
Fig. 4 Schematic illustration of synthesis process of Mn-Ce binary oxide by sol-gel method
图5 (A)CeO2纳米棒负载MnO2纳米片异质结构的合成示意图;(B, C)SEM和HRTEM图[27]
Fig. 5 (A) Schematic illustration of synthesis process and(B, C) SEM and high resolution TEM images of CeO2 nanowire/MnO2 nanosheet heterogeneous structure[27]
图6 (A)Mn3O4/CeO2纳米管的合成示意图; (B, C)Mn3O4/CeO2纳米管的FESEM和TEM图[33]
Fig. 6 (A) Schematic illustration of synthesis process and(B, C) FESEM and TEM images of Mn3O4/CeO2 nanotubes[33]
图7 (A, B)MnxCe1-xO2的SEM图[40]
Fig. 7 (A, B) SEM images of MnxCe1-xO2[40]
图8 (A)SAS的工艺流程图;(B,C)空心和实心MnOx-CeO2纳米球的HRTEM图[41]
Fig. 8 (A) Schematic diagram of SAS apparatus;(B,C) High resolution TEM images of hollow and solid MnOx-CeO2 nanospheres[41]
表2 不同方法制备产物的催化性能和物化性质[51]
Table 2 Catalytic performance and physicochemical properties of different products[51]
Method NO conversion
(200 ℃)/%		 N2 selectivity
(200 ℃)/%		 Acid amount(α+β)/a.u. Atom ratio/%
Ce3+/(Ce3++Ce4+) Mn4+/(Mn2++Mn3++Mn4+) Oabs/(Olat+Oabs)
MMM 25 72 1978 13.98 22.93 30.02
CPM 90 60 3611 16.29 28.13 32.19
IM 75 60 2957 15.42 31.62 31.38
SGM 96 71 4475 17.57 29.80 33.79
HTM 100 71 6021 18.67 41.65 36.50
图9 (A, B)中空MnOx-CeO2纳米管催化剂的SEM和TEM图;催化剂的(C)NOx的转化率和(D)N2的选择性[54]
Fig. 9 (A, B)SEM and TEM images of hollow MnOx-CeO2 nanotubes;(C) NOx conversion and(D) N2 selectivity of catalysts[54]
图10 (A)不同Ce/Ti比材料的示意图;复合催化剂的(B)NOx的转化率和(C)耐受性[57]
Fig. 10 (A) Schematic diagram;(B) NOx conversion and (C) tolerance of catalysts with different Ce/Ti ratios[57]
图11 (A)不同Ce/Mn比催化剂的苯转化率;(B)Ce0.3Mn0.7O2的TEM图;(C)CexMn1-xO2上苯催化氧化的机理图[25]
Fig. 11 (A) Benzene conversion of catalysts with different Ce/Mn ratios;(B) TEM image of Ce0.3Mn0.7O2;(C) The mechanism of benzene catalytic oxidation over CexMn1-xO2[25]
图12 Mn0.8Ce0.2O2/HZSM-5的(A)氯苯转化率;(B)反应模型图;(C)反应机理图[87,88]
Fig. 12 (A) Chlorobenzene conversion;(B) Schematic diagram of reaction models and (C) Reaction mechanism of Mn0.8Ce0.2O2/HZSM-5[87,88]
图13 碳烟氧化过程中的氧空位的形成示意图[104]
Fig. 13 Schematic diagram of evolution of oxygen vacancies in soot catalytic oxidation[104]
图14 6%Ce-6%MnOx/Ti-PILC共同催化NH3-SCR脱硝和Hg0氧化的机理图[152]
Fig. 14 Reaction mechanism for NH3-SCR and Hg0 oxidation of 6%Ce-6%MnOx/Ti-PILC[152]
表3 Mn-Ce二元氧化物对大气污染物的消除
Table 3 Abatement of atmospheric pollutants by Mn-Ce binary oxides
Catalyst Pollutant Testing condition Catalytic performance
/℃(Tx)*		 Synthesis method ref
MnOx-CeO2
hollownanotube		 NOx 1000 ppm NOx, 1000 ppm NH3,
5% O2, 10% H2O, N2 balance,
GHSV=30 000 h-1		 100(T100) Template method 54
Mn-CeOx/CNTs NOx 500 ppm NO, 500 ppm NH3, 5% O2,
N2 balance, GHSV=210 000 h-1		 120(T90) Redox method 65
PdO/CeO2-MnOx Benzene 1000 ppm benzene, 20% O2,
N2 balance, 100 mg catalysts, WHSV=60 000 h-1		 250(T100) Hydrothermal and
precipitation methods		 84
Mn0.85Ce0.15O2 nanorod Toluene 1000 ppm toluene, 20% O2,
N2 balance, 300 mg catalysts, WHSV=32 000 h-1		 225(T100) Hydrothermal method 85
Mn0.8Ce0.2O2/HZSM-5 Chlorobenzene 1000 ppm chlorobenzene, 10% O2,
N2 balance, 1000 mg catalysts,
GHSV=10 000 h-1		 Dry: 250
Humid: 280
(T100)		 Hydrothermal and
impregnant methods		 87
Ce0.93Mn0.07Ox nanosphere CO 1% CO, 10% O2, N2 balance
30 mg catalysts, 40 mL·min-1		 255(T100) Hydrothermal method 116
MnOx-CeO2 solid solution HCHO 580 ppm HCHO, 18% O2,
He balance, GHSV=21 000 h-1		 100(T100) Coprecipitation method 130
6%Ce-6%MnOx/Ti-PILC Hg0, NO 500 ppm NO, 500 ppm NH3, 5% O2,
50 μg·m-3 Hg0, N2 balance,
500 mg catalysts,GHSV=50 000 h-1		 Hg0 & NO
200(T95)		 Impregnation method 37
图15 Mn0.3Ce0.7O2的(A)极化曲线;(B)200 mA·cm-2恒流放电曲线[156]
Fig. 15 (A)The linear polarization curves and (B)galvanostatic discharge curves at 200 mA·cm-2 of Mn0.3Ce0.7O2 catalyst[156]
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锰铈二元氧化物的制备与应用