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组成对用于CO加氢合成二甲醚的CuO-ZnO-AlO/HZSM-5杂化材料功能的影响

The influence of composition on the functionality of hybrid CuO-ZnO-AlO/HZSM-5 for the synthesis of DME from CO hydrogenation.

作者信息

Hu Yubing, Zhang Yajing, Du Jie, Li Chunyan, Wang Kangjun, Liu Lidong, Yu Xinrui, Wang Kai, Liu Nan

机构信息

College of Chemical Engineering, Shenyang University of Chemical Technology Shenyang 110142 PR China

出版信息

RSC Adv. 2018 Aug 28;8(53):30387-30395. doi: 10.1039/c8ra04814b. eCollection 2018 Aug 24.

Abstract

A series of CuO-ZnO-AlO/HZSM-5 hybrid catalysts with different Cu/Zn ratios and disparate AlO doping were prepared and characterized by XRD, BET, H-TPR, NH-TPD and XPS techniques. The optimal Cu/Zn ratio is 7 : 3, and the introduction of a suitable amount of AlO to form hybrid catalysts increased the BET specific area and micropore volume, facilitated the CuO dispersion, decreased the CuO crystallite size, increased the interaction between CuO and ZnO, enhanced the number of weak acid sites, altered the copper chemical state and improved the catalytic performance consequently. The highest CO conversion, DME selectivity and DME yield of 27.3%, 67.1% and 18.3%, respectively, were observed over the CZAH catalyst. The suitable temperature of 260 °C and the appropriate space velocity of 1500 h for one-step synthesis of dimethyl ether (DME) from carbon dioxide (CO) hydrogenation were also investigated. The 50 h stability of the CZAH catalyst was also tested.

摘要

制备了一系列具有不同铜锌比和不同氧化铝掺杂量的CuO-ZnO-AlO/HZSM-5混合催化剂,并采用XRD、BET、H-TPR、NH-TPD和XPS技术对其进行了表征。最佳铜锌比为7:3,引入适量的氧化铝形成混合催化剂增加了BET比表面积和微孔体积,促进了CuO的分散,减小了CuO微晶尺寸,增强了CuO与ZnO之间的相互作用,增加了弱酸位点的数量,改变了铜的化学状态,从而提高了催化性能。在CZAH催化剂上观察到最高的CO转化率、二甲醚选择性和二甲醚产率分别为27.3%、67.1%和18.3%。还研究了由二氧化碳(CO)加氢一步合成二甲醚(DME)的合适温度260℃和合适空速1500 h⁻¹。同时测试了CZAH催化剂的50 h稳定性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a9c4/9085472/faf69fceeb2f/c8ra04814b-f1.jpg

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