Modification of acid–base properties of metal-doped ZnO catalysts for the transesterification of propylene carbonate with methanol to dimethyl carbonate

IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Pimchanok Ieamviteevanich, Pattaraporn Kim-Lohsoontorn, Panpailin Seeharaj
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Abstract

This study investigated the effect of metal dopants on the surface properties of ZnO-based catalysts for the transesterification of propylene carbonate (PC) with methanol to produce dimethyl carbonate (DMC). A series of metal-doped ZnO nanocatalysts (M-ZnO, where M is Ca2+, Cu2+, Ce3+, La3+, and Y3+ with the mol ratio of Zn2+/Mx+  = 4) were prepared by a simple co-precipitation method followed by calcining in air at 673 K for 5 h. Introducing different metal cations into the ZnO system decreased crystallite size and created surface defects of exposed cations and oxygen vacancies, increasing surface-active acid and basic sites. The catalytic performance for DMC production was ranked as follows: Ca-ZnO < Cu–ZnO < ZnO < Ce-ZnO < Y-ZnO < La-ZnO. La-ZnO showed the highest performance of all catalysts, with 67% PC conversion, 67% DMC selectivity, and 45% DMC yield. The improvement of catalytic activity was correlated with an increase in the concentration of moderate and strong acid–base functionalities on the La-ZnO surfaces for participating in the reaction of PC and methanol to form DMC.

Graphic abstract

金属掺杂氧化锌催化剂对碳酸丙烯与甲醇酯交换制碳酸二甲酯酸碱性质的改性
研究了金属掺杂剂对氧化锆基催化剂表面性能的影响。氧化锆基催化剂用于碳酸丙烯(PC)与甲醇酯交换制备碳酸二甲酯(DMC)。采用共沉淀法制备了一系列金属掺杂ZnO纳米催化剂(M-ZnO,其中M为Ca2+、Cu2+、Ce3+、La3+和Y3+, Zn2+/Mx+的摩尔比为4),并在673 K空气中煅烧5 h。在ZnO体系中引入不同的金属阳离子,可以减小晶粒尺寸,产生暴露阳离子的表面缺陷和氧空位,增加表面活性酸碱位。对DMC的催化性能排序为:Ca-ZnO <、Cu-ZnO <、ZnO <、Ce-ZnO <、Y-ZnO <、La-ZnO。在所有催化剂中,La-ZnO表现出最高的性能,PC转化率为67%,DMC选择性为67%,DMC产率为45%。催化活性的提高与La-ZnO表面参与PC与甲醇反应生成DMC的中、强酸碱官能团浓度的增加有关。图形抽象
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来源期刊
CiteScore
5.70
自引率
18.20%
发文量
229
审稿时长
2.6 months
期刊介绍: Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry. The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.
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