Effect of mesoporous construction on catalytic performance of CuY methanol oxidative carbonylation

被引：0

作者：

Liang J. ^{[1
]}

Zhang G. ^{[1
]}

Gao Y. ^{[2
]}

Yin J. ^{[1
]}

Zheng H. ^{[1
]}

Li Z. ^{[1
]}

机构：

[1] Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan

[2] Luan Chemical Group Co., Ltd., Changzhi

来源：

Huagong Xuebao/CIESC Journal | 2021年 / 72卷 / 09期

关键词：

Catalyst; Cu[!sup]+[!/sup] active sites; Mesopore; Oxidative carbonylation; Zeolite;

D O I：

10.11949/0438-1157.20201937

中图分类号：

学科分类号：

摘要：

H4EDTA, H2Na2EDTA and NaOH aqueous solutions were used to modify the original NaY zeolite separately by acid-base modification and continuous acid-base modification, and the corresponding CuY catalyst was prepared by the liquid-phase ion exchange method. The N2-physisorption, TEM, XRD, 29Si NMR, 27Al NMR, NH3-TPD, Py-IR, ICP, XPS and CO-FTIR were used to characterize the structure of the support and catalyst. The effect of mesoporous construction in NaY zeolite on catalytic performance of CuY for oxidative carbonylation of methanol was investigated. The results indicated that partial framework Al of NaY zeolite were extracted after sole treatment by H4EDTA, with the formation of extra-framework Si and Al species, and the obtained E-NaY did not form obvious mesoporous. Extra-framework and partial framework Al of E-NaY zeolite were removed after acid washing by H2Na2EDTA, and the obtained EW-NaY generated obvious mesoporous. The extracted Al species were reinserted back into the framework of zeolite accompanied with desilication during alkali treatment of E-NaY and EW-NaY by 0.2 mol/L NaOH, and abundant mesopores were formed in the obtained E0.2AT-NaY and EW0.2AT-NaY zeolite. Moreover, the utilization of exchanged sites for Cu+ accessible to reactants for EW0.2AT-NaY attained the maximum due to the highest mesopore volume (0.45 cm3/g) and abundant Al-defects structure. Nevertheless, the number of exchanged sites for Cu+ (66 μmol/g) accessible to reactants was significantly less than that of E0.2AT-NaY (176 μmol/g) due to higher dealumination degree of EW0.2AT-NaY than that of E0.2AT-NaY. Consequently, the number of Cu+ active sites and catalytic activity for EW0.2AT-CuY were just slightly lower than that for E0.2AT-CuY, and the catalytic activities for both were about 2.2 times as that of the pristine CuY catalyst. © 2021, Editorial Board of CIESC Journal. All right reserved.

引用

页码：4685 / 4697

页数：12

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