Effect of Mg modification on the catalytic performance of zinc malachite for methanol synthesis

Q3 Energy 燃料化学学报 Pub Date : 2024-09-01 DOI:10.1016/S1872-5813(24)60455-X
YUAN Zhiguo , ZHANG Fan , YANG Shili , XU Xiaoying , LIU Chenyang , QIU Zhengpu , WEI Wei
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Abstract

The complex conditions of methanol production from coke-oven gas have brought challenges to the copper-based methanol synthesis catalyst. In this work, a series of zinc-malachite samples with different Mg contents were prepared. The zinc-malachite and calcined samples were characterized by in-situ X-ray diffraction (XRD), thermogravimetry-mass spectrometry (TG-MS), N2 physical adsorption, H2 programmed temperature reduction (H2-TPR), CO2 programmed temperature desorption (CO2-TPD) and other methods. The effects of Mg addition on the structure of zinc-malachite and its catalytic performance of methanol synthesis were investigated. The results showed that the addition of Mg increased the degree of Cu substitution inside the zinc-malachite structure and promoted the formation of high temperature carbonates in the catalyst after roasting. With the increase of Mg content, the specific surface area of the calcined catalyst increased gradually, and the Cu grain size decreased simultaneously. In-situ XRD results showed that a small amount of Mg could effectively inhibit the growth of copper grain size during the heat treatment. The evaluation showed that the initial activity of the catalyst increased first and then decreased with Mg addition, and the activity of the Mg-doped catalyst remained at a relatively high level after heat treatment. The appropriate Mg addition is beneficial to the initial activity and thermal stability of Cu-based methanol synthesis catalyst.

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镁改性对用于甲醇合成的孔雀石锌催化性能的影响
利用焦炉煤气生产甲醇的复杂条件给铜基甲醇合成催化剂带来了挑战。本研究制备了一系列不同镁含量的锌-孔雀石样品。通过原位 X 射线衍射 (XRD)、热重质谱 (TG-MS)、N2 物理吸附、H2 程序温度还原 (H2-TPR)、CO2 程序温度解吸 (CO2-TPD) 等方法对锌-孔雀石和煅烧样品进行了表征。研究了添加镁对锌-孔雀石结构及其甲醇合成催化性能的影响。结果表明,镁的加入增加了锌-孔雀石结构内部铜的取代程度,促进了焙烧后催化剂中高温碳酸盐的形成。随着镁含量的增加,煅烧催化剂的比表面积逐渐增大,铜晶粒尺寸同时减小。原位 XRD 结果表明,少量的镁能有效抑制热处理过程中铜晶粒的长大。评估结果表明,随着镁的添加,催化剂的初始活性先升高后降低,掺杂镁的催化剂在热处理后活性仍保持在较高水平。适当添加镁有利于提高铜基甲醇合成催化剂的初始活性和热稳定性。
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来源期刊
燃料化学学报
燃料化学学报 Chemical Engineering-Chemical Engineering (all)
CiteScore
2.80
自引率
0.00%
发文量
5825
期刊介绍: Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.
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