Surface Properties of Ce1-xMnxO2 Catalyst on the Catalytic Activities for Direct Synthesis of DMC from CO2 and Methanol

doi:10.7503/cjcu20200250

Abstract

Abstract:

A series of Ce_1-_xMn_xO₂ catalysts with different Mn doping amounts were prepared by coprecipitation method and applied to catalyze direct synthesis of dimethyl carbonate(DMC) from CO₂ and methanol. The effects of surface properties of Ce_1-_xMn_xO₂ on the direct synthesis of DMC from CO₂ and methanol were studied by means of X-ray diffraction(XRD), N₂ adsorption-desorption, transmission electron microscopy(TEM), X-ray photoelectron spectroscopy(XPS) and programmed temperature desorption(TPD). The results indicated that Mn ions successfully entered into the lattice of CeO₂ and formed a uniform solid solution. With the increase of Mn doping, the number of weak acid and base sites on the catalyst surface decreased gradually, while the number of medium and strong acid and base sites increased. Meanwhile, the oxygen vacancy content on the catalyst surface increased first and then decreased with the increase of Mn doping. When the doping of Mn was low, the ratio of Mn²⁺ on the catalyst surface was high, which was beneficial for the reaction of Ce⁴⁺+ Mn²⁺→Ce³⁺+ Mn³⁺ and the formation of oxygen vacancies. With further increase of Mn doping, the ratio of Mn⁴⁺ on the catalyst surface increase, which was conducive to the reaction of Ce³⁺+Mn⁴⁺→Ce⁴⁺+Mn³⁺, resulting in the decrease of oxygen vacancy. The catalytic activity of Ce_1-_xMn_xO₂ catalyst was linearly correlated with the content of oxygen vacancy on surface.

Key words: Carbon dioxide, Dimethyl carbonate(DMC), Catalyst, Acidity-basicity property, Oxygen vacancy

CLC Number:

O643

TrendMD:

ZHANG Guoqiang, SUN Yuchen, SHI Yabo, ZHENG Huayan, LI Zhong, SHANGGUAN Ju, LIU Shoujun, SHI Pengzheng. Surface Properties of Ce_1-_xMn_xO₂ Catalyst on the Catalytic Activities for Direct Synthesis of DMC from CO₂ and Methanol[J]. Chem. J. Chinese Universities, 2020, 41(9): 2061.

Figures/Tables 14

References 52

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Sample	2θ/(°)	Interplanar spacing/nm	Lattice parameter/nm	Particle size^*/nm
CeO₂	28.50	0.31293	0.54201	10.106
Ce_0.983Mn_0.017O₂	28.53	0.31260	0.54145	10.326
Ce_0.956Mn_0.044O₂	28.55	0.31250	0.54126	9.570
Ce_0.91Mn_0.09O₂	28.58	0.31239	0.54108	8.782
Ce_0.864Mn_0.136O₂	28.61	0.31207	0.54052	8.987

Sample	2θ/(°)	Interplanar spacing/nm	Lattice parameter/nm	Particle size^*/nm
CeO₂	28.50	0.31293	0.54201	10.106
Ce_0.983Mn_0.017O₂	28.53	0.31260	0.54145	10.326
Ce_0.956Mn_0.044O₂	28.55	0.31250	0.54126	9.570
Ce_0.91Mn_0.09O₂	28.58	0.31239	0.54108	8.782
Ce_0.864Mn_0.136O₂	28.61	0.31207	0.54052	8.987

Catalyst	S_BET/(m²·g^-1)	V_p/(cm³·g^-1)	Pore size/nm
CeO₂	145	0.60	11.6
Ce_0.983Mn_0.017O₂	145	0.62	12.2
Ce_0.956Mn_0.044O₂	147	0.58	11.1
Ce_0.910Mn_0.090O₂	145	0.63	12.0
Ce_0.864Mn_0.136O₂	147	0.68	12.8

Catalyst	S_BET/(m²·g^-1)	V_p/(cm³·g^-1)	Pore size/nm
CeO₂	145	0.60	11.6
Ce_0.983Mn_0.017O₂	145	0.62	12.2
Ce_0.956Mn_0.044O₂	147	0.58	11.1
Ce_0.910Mn_0.090O₂	145	0.63	12.0
Ce_0.864Mn_0.136O₂	147	0.68	12.8

Sample	CO₂ adsorption^a/(mmol·g^-1)			NH₃ adsorption^b/(mmol·g^-1)
Sample	Weak(<200 ℃)	Moderate(200―400 ℃)	Strong(>400 ℃)	Weak(<200 ℃)	Moderate(200―400 ℃)	Strong(>400 ℃)
CeO₂	0.226	0.046	0.017	0.723	0.027	0.048
Ce_0.983Mn_0.017O₂	0.156	0.072	0.020	0.549	0.057	0.036
Ce_0.956Mn_0.044O₂	0.141	0.075	0.032	0.204	0.094	0.038
Ce_0.910Mn_0.090O₂	0.121	0.110	0.036	0.186	0.140	0.056
Ce_0.864Mn_0.136O₂	0.102	0.120	0.047	0.220	0.134	0.064

Surface Properties of Ce_1-_xMn_xO₂ Catalyst on the Catalytic Activities for Direct Synthesis of DMC from CO₂ and Methanol

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Catalyst	Molar fraction(%)
Catalyst	Ce³⁺	Ce⁴⁺	O_V	Mn⁴⁺	Mn³⁺	Mn²⁺
CeO₂	10.8	89.2	5.6	—	—	—
Ce_0.983Mn_0.017O₂	14.6	85.4	6.9	8.8	76.8	14.3
Ce_0.956Mn_0.044O₂	11.1	88.9	6.2	12.5	76.4	11.1
Ce_0.910Mn_0.090O₂	10.7	89.3	4.9	15.7	77.2	7.1
Ce_0.864Mn_0.136O₂	9.8	90.2	4.5	19.4	73.5	7.1

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