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Progress in Chemistry 2019, Vol. 31 Issue (6): 811-830 DOI: 10.7536/PC181042 Previous Articles   Next Articles

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: Online: Published:
  • 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)
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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
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
Fig. 1 Crystal structure of CeO2
Fig. 2 Schematic illustration of synthesis process and SEM image of flower like Mn-doped CeO2[16]
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]
Fig. 4 Schematic illustration of synthesis process of Mn-Ce binary oxide by sol-gel method
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]
Fig. 6 (A) Schematic illustration of synthesis process and(B, C) FESEM and TEM images of Mn3O4/CeO2 nanotubes[33]
Fig. 7 (A, B) SEM images of MnxCe1-xO2[40]
Fig. 8 (A) Schematic diagram of SAS apparatus;(B,C) High resolution TEM images of hollow and solid MnOx-CeO2 nanospheres[41]
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
Fig. 9 (A, B)SEM and TEM images of hollow MnOx-CeO2 nanotubes;(C) NOx conversion and(D) N2 selectivity of catalysts[54]
Fig. 10 (A) Schematic diagram;(B) NOx conversion and (C) tolerance of catalysts with different Ce/Ti ratios[57]
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]
Fig. 12 (A) Chlorobenzene conversion;(B) Schematic diagram of reaction models and (C) Reaction mechanism of Mn0.8Ce0.2O2/HZSM-5[87,88]
Fig. 13 Schematic diagram of evolution of oxygen vacancies in soot catalytic oxidation[104]
Fig. 14 Reaction mechanism for NH3-SCR and Hg0 oxidation of 6%Ce-6%MnOx/Ti-PILC[152]
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
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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