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A novel microreaction strategy to fabricate superior hybrid zirconium and zinc oxides for methanol synthesis from CO2
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2020-03-02 , DOI: 10.1016/j.apcata.2020.117507
Xiuxiu Wang , Yizhou Wang , Chunliang Yang , Yun Yi , Xiaodan Wang , Fei Liu , Jianxin Cao , Hongyan Pan

The synergetic interaction of solid solutions plays important roles in the reaction efficiency of CO2 hydrogenation, which is used to produce methanol. The effects of material mixing, impregnation, traditional coprecipitation, and microreaction synthesis on the structural and catalytic properties of ZnO/t-ZrO2 hybrid oxides were investigated. Although the impregnation effect caused a certain electronic structural modulation at the Zn/Zr interface, the pore structure blocking effect and low number of oxygen vacancy defects leaded to a low catalytic reaction efficiency. The solid solution structure enhanced the Zn/Zr interfacial interaction and increased the electron binding energy. More importantly, many oxygen vacancy defects were formed, which promoted CO2 activation. However, the solid solution structure was more affected by the preparation method. The solid solution formed from the microreaction exhibited excellent catalytic activity, thermal stability and regeneration performance due to a more uniform solid solution structure and abundant oxygen vacancy defects. The CO2 conversion rate, methanol selectivity, and methanol space-time yield (STY) under the conditions of H2/CO2 = 3:1, 320 °C, 3 MPa, GHSV = 12000 ml g-1 h-1 reached 9.2%, 93.1%, and 0.35 gMeOH h-1gcat-1, respectively.



中文翻译:

一种新颖的微反应策略,可制备用于从CO 2合成甲醇的高级杂化锆和氧化锌

固溶体的协同相互作用在用于生产甲醇的CO 2加氢反应效率中起着重要作用。研究了材料混合,浸渍,传统的共沉淀和微反应合成对ZnO / t-ZrO 2杂化氧化物的结构和催化性能的影响。尽管浸渍作用在Zn / Zr界面上引起了一定的电子结构调节,但是孔结构的阻断作用和氧空位缺陷的数量少导致催化反应效率低。固溶体结构增强了Zn / Zr界面相互作用并增加了电子结合能。更重要的是,形成了许多氧空位缺陷,从而促进了CO 2激活。然而,固溶体结构受制备方法的影响更大。由于更均匀的固溶体结构和大量的氧空位缺陷,由微反应形成的固溶体表现出优异的催化活性,热稳定性和再生性能。该CO 2的转化率,甲醇的选择性,及H的条件下,甲醇的时空产率(STY)2 / CO 2  = 3:1,320℃,3MPa的,GHSV =12000毫升克-1  ħ -1达到分别为9.2%,93.1%和0.35 g MeOH  h -1 g cat -1

更新日期:2020-03-03
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