Advantage of microreactor on the synthesis of high-activity Cu-Mn catalyst by co-precipitation

doi:10.11949/0438-1157.20221575

Abstract

Abstract:

Cu-Mn coprecipitates with different copper manganese molar ratios were synthesised by co-precipitation method in the Caterpillar microreactor, and Cu-Mn composite oxide catalysts were prepared after calcining. The phase and structure of the precipitates and catalysts were analyzed by X-ray diffraction (XRD), thermogravimetric analysis (TG), Raman spectroscopy (Raman spectrum) and X-ray photoelectron spectroscopy (XPS). The results show that with the content of Cu increasing, the proportion of Mn³⁺ in the catalyst decreased gradually, the content of the surface lattice oxygen increased first and then decreased, and the catalytic performance of oxidation of toluene increased first and then decreased. The flow reaction characteristics of microreactor make Cu and Mn element in the catalyst maintain good dispersion, which contributes to increasing the content of Mn³⁺ in the catalyst. On the basis of high Mn³⁺ catalyst, the surface lattice oxygen becomes the dominating factor of catalytic performance.

Key words: microreactor, precipitation, copper manganese molar ratio, copper manganese compound oxide, catalyst

摘要：

在Caterpillar微反应器中采用共沉淀法制备了不同铜锰比的共沉淀物，直接焙烧得到铜锰复合氧化物催化剂。采用X射线衍射(XRD)、热重分析(TG)、拉曼光谱(Raman)和X射线光电子能谱(XPS)对沉淀物和催化剂进行了物相和结构分析。结果显示，随着Cu含量的增加，催化剂中Mn³⁺所占比例逐渐下降，表面晶格氧含量呈现先上升后下降的趋势，催化甲苯降解的活性呈现先上升后下降的规律。微反应器中的流动反应特性使得催化剂中的Cu、Mn保持良好分散性，有利于提高催化剂中Mn³⁺含量，此时表面晶格氧成为催化活性的制约因素。

关键词: 微反应器, 沉淀, 铜锰配比, 铜锰复合氧化物, 催化剂

CLC Number:

TQ 426.6

Jiawei FU, Shuaishuai CHEN, Kailun FANG, Xin JIANG. Advantage of microreactor on the synthesis of high-activity Cu-Mn catalyst by co-precipitation[J]. CIESC Journal, 2023, 74(2): 776-783.

付家崴, 陈帅帅, 方凯伦, 蒋新. 微反应器共沉淀反应制备铜锰催化剂[J]. 化工学报, 2023, 74(2): 776-783.

Figures/Tables 12

Fig.1 Flow diagram of preparation process and structure of microreactor

Fig.2 Schematic diagram of catalytic process for Cu-Mn catalyst

Fig.3 Effect of Cu content in catalyst on catalytic degradation of toluene

Fig.4 XRD patterns of precipitates with different ratios of Cu to Mn

Fig.5 TG-MS curves of the precipitates

Fig.6 DTG curves of Cu-Mn precipitates

Fig.7 XRD patterns of Cu-Mn catalysts

Fig.8 Raman spectra of Cu-Mn catalysts

Fig.9 XPS spectra of Cu-Mn catalysts

Table 1 Surface species content of catalyst based on XPS spectra

催化剂	O_latt/O_ads	Mn³⁺/Mn⁴⁺	Cu⁺/Cu²⁺
Cu_0.1Mn_0.9	1.36	2.25	0.20
Cu_0.2Mn_0.8	1.76	2.16	0.81
Cu_0.3Mn_0.7	1.96	1.94	0.08
Cu_0.4Mn_0.6	0.72	1.47	0
Cu_0.5Mn_0.5	0.65	1.14	0

Fig.10 Surface species variation trend of Cu-Mn catalyst

Fig.11 T90 activity of Cu-Mn catalysts with different Mn3+ and Olatt

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