前驱体转化法可控制备γ-二氧化锰及其催化燃烧甲苯性能

doi:10.19964/j.issn.1006-4990.2021-0696

Abstract

Abstract:

Three groups of γ-MnO₂ catalysts（Mn-N，Mn-S，Mn-A） were prepared by disproportionation reaction between Mn₃O₄ and nitric acid，sulfuric acid，and acetic acid，respectively.The effect of different acid on the structure and morphology of the products was studied.The physical and chemical properties of the products were systematically analyzed by X-ray diffraction（XRD），scanning electron microscopy（FE-SEM），transmission electron microscopy（HR-TEM），nitrogen adsorption desorption，X-ray photoelectron spectroscopy（XPS），hydrogen temperature programmed reduction（H₂-TPR） and oxygen temperature programmed desorption（O₂-TPD）.And toluene catalytic combustion was used as a probe reaction to evaluate the activity of γ-MnO₂ catalyst.The results showed that the catalyst Mn-N treated with nitric acid had the best catalytic combustion activity for toluene.Under the condition of mass space velocity of 40 000 mL/（g·h），the ignition temperature T₁₀（corresponding conversion of 10%） was 190 ℃，and the complete combustion temperature T₉₀（corresponding conversion of 90%） was 229 ℃.This may be related to its large specific surface area，high content of Mn（Ⅲ） and adsorbed oxygen species，good reducibility and lattice oxygen flow ability.In addition，Mn-N could still maintain good catalytic activity after continuous stability experiments for 30 h.

Key words: precursor conversion, Mn₃O₄, γ-MnO₂, toluene, catalytic combustion

CLC Number:

TQ137.12

TANG Shichang,CHENG Gao,LIU Qi,YE Fan,SUN Ming,YU Lin. Controllable preparation of γ-MnO₂ by precursor conversion method and its catalytic combustion performance of toluene[J]. Inorganic Chemicals Industry, 2022, 54(6): 134-141.

Figures/Tables 10

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Table 1

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样品	比表面积/ （m²·g^-1）	平均孔径/ nm	催化燃烧甲苯活性		n（Mn³⁺）/ n（Mn⁴⁺）	n（O_A）/ n（O_L）	H₂-TPR 峰/℃	O₂-TPD 峰/℃
样品	比表面积/ （m²·g^-1）	平均孔径/ nm	T₁₀/℃	T₉₀/℃	n（Mn³⁺）/ n（Mn⁴⁺）	n（O_A）/ n（O_L）	H₂-TPR 峰/℃	O₂-TPD 峰/℃
Mn-N	155.2	17.36	190	229	1.70	1.15	217	441
Mn-S	82.0	17.50	203	237	1.58	0.96	240	464
Mn-A	115.2	23.56	211	258	1.13	0.77	248	487

样品	反应条件		催化燃烧甲苯活性
样品	甲苯体积分数/10^-6	空速/ （mL·g^-1·h^-1）	T₁₀/℃	T₉₀/℃
花状ε-MnO₂^［19］	1 000	40 000	217	280
棒状α-MnO₂^［20］	1 000	21 000	220	250
Mn10Cu1-S^［21］	1 000	15 000	210	258
10%MnO _x /HZSM-5-25^［22］	1 000	24 000	220	261
2%Co₃O₄/3DOM LSCO^［23］	1 000	21 000	190	243
Co₃O₄-400^［24］	1 000	20 000	218	259
Co₃O₄-KIT-6^［25］	1 000	15 000	203	233
5.8%Au/3DOM Mn₂O₃^［26］	1 000	40 000	211	244
6.5Au/3DOM Co₃O₄^［27］	1 000	40 000	215	256
Mn-N（制备样品）	1 000	40 000	190	229

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Controllable preparation of γ-MnO₂ by precursor conversion method and its catalytic combustion performance of toluene

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Controllable preparation of γ-MnO2 by precursor conversion method and its catalytic combustion performance of toluene