一种合成Cu-ZnO共沉淀催化剂的新方法及其高温甲醇分解活性

IF 0.6 4区 工程技术 Q4 ENERGY & FUELS Journal of The Japan Petroleum Institute Pub Date : 2021-05-01 DOI:10.1627/JPI.64.132
H. Saima, Masatoshi Todaka, Kono Tatsuya, R. Maruta, Kodai Kadota, Y. Mogi
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引用次数: 0

摘要

温室气体特别是二氧化碳排放增加导致的全球变暖是一个紧迫的全球性问题。大气二氧化碳浓度在2015年上升到400ppm1以上,并且还在继续增加。因此,必须大幅减少或完全消除二氧化碳的排放,以防止到21002年全球气温上升超过2摄氏度。一种解决方案是利用可再生能源产生的氢气将二氧化碳回收为燃料。以前的研究已经检验了从二氧化碳中合成碳氢化合物,如甲烷、甲醇、汽油和柴油。CO2可有效合成甲烷和甲醇;但是甲醇的产率受到反应的热力学平衡的强烈限制。例如,4mpa时合成气的甲醇收率在473 K时仅为30%,在523 K时仅为13%。甲醇转化为二甲醚(DME)可提高甲醇和二甲醚的收率。以γ-Al2O3为催化剂,在543 K条件下,甲醇和二甲醚的收率最高,为24%。类似的可能性可以应用于将二氧化碳转化为碳氢化合物,这是目前更重要的燃料。其他研究报道了由合成气4)~6)合成碳氢化合物。在623 K和2.1 MPa条件下,采用CuZnO和超稳定y型沸石催化剂组合反应,得到了30%的烃类收率,其中约75%为C3和C4石蜡,或液化石油气(LPG)。这些技术可以应用于从二氧化碳合成碳氢化合物;而CuZnOAl2O3等甲醇合成催化剂在沸石催化剂活性生成甲醇/二甲醚烃的条件下热稳定性较低。因此,需要开发一种具有高热稳定性的新型甲醇合成催化剂。小于100 μm的细气泡表现出独特的行为。细气泡具有较大的比表面积,因此气泡内的气体分子会容易而迅速地与周围的液体接触。本文介绍了一种用细气泡通过溶液制备沉淀催化剂的新方法。混合金属盐溶液会在细气泡中迅速与氨反应,但生成的金属氢氧化物不太可能聚集成大颗粒,因为沉淀只在液体和细气泡的界面上产生。因此,用这种细泡法制备的沉淀物的颗粒直径被认为是非常细的,具有很大的比表面积。用[普通纸]制备CuZnOAl2O3催化剂
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A New Method for Synthesizing Co-precipitated Cu–ZnO Catalyst and Its Activity for Methanol Decomposition at High Temperature
Global warming caused by increased emissions of greenhouse gases, especially CO2, is a pressing global problem. Atmospheric CO2 concentration rose above 400 ppm1) in 2015, and continues to increase. Therefore, CO2 emissions must be drastically reduced or eliminated entirely to prevent an increase in global temperature of more than 2 K by 21002). One solution is to recycle CO2 into fuel using hydrogen produced from renewable energy sources. Previous studies have examined the synthesis of hydrocarbons such as methane, methanol, gasoline, and diesel fuel from CO2. Methane and methanol can be effectively synthesized from CO2; but the methanol yield is strongly limited by the thermodynamic equilibrium of the reaction. For example, the yield of methanol from synthesis gas at 4 MPa is only 30 % at 473 K, and 13 % at 523 K. Conversion of methanol to dimethyl ether (DME) may increase the yield of methanol and DME3). The highest yield of methanol and DME was 24 % at 543 K, achieved by combining a methanol synthesis catalyst with γ-Al2O3. Similar possibilities can be applied to the conversion of CO2 to hydrocarbons, which are currently a more important fuel. Other studies have reported hydrocarbon synthesis from syngas4)~6). Use of a combination of CuZnO and ultra-stable Y-type zeolite catalyst at 623 K and 2.1 MPa obtained a yield of hydrocarbons of 30 %, about 75 % of which were C3 and C4 paraffins, or liquefied petroleum gas (LPG). These techniques can be applied to hydrocarbon synthesis from CO2; but methanol synthesis catalysts such as CuZnOAl2O3 have low thermal stabilities at the conditions under which the zeolite catalyst actively forms hydrocarbons from methanol/dimethyl ether. Therefore, development of a new methanol synthesis catalyst with high thermal stability is required. Fine bubbles smaller than 100 μm show unique behavior. Fine bubbles have a large specific surface area, so gas molecules inside the bubble will easily and rapidly contact with the surrounding liquid. Here we describe a new method for the preparation of precipitated catalyst by passing fine bubbles through a solution. Mixed metal salts solution will quickly react with ammonia in fine bubbles but the resulting metal hydroxide is unlikely to aggregate into large particles because the precipitate is generated only at the interface of the liquid and fine bubbles. Consequently, the particle diameter of the precipitate prepared by this fine bubble method is thought to be very fine with a large specific surface area. A CuZnOAl2O3 catalyst, prepared with [Regular Paper]
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来源期刊
Journal of The Japan Petroleum Institute
Journal of The Japan Petroleum Institute 工程技术-工程:石油
CiteScore
1.70
自引率
10.00%
发文量
29
审稿时长
>12 weeks
期刊介绍: “Journal of the Japan Petroleum Institute”publishes articles on petroleum exploration, petroleum refining, petrochemicals and relevant subjects (such as natural gas, coal and so on). Papers published in this journal are also put out as the electronic journal editions on the web. Topics may range from fundamentals to applications. The latter may deal with a variety of subjects, such as: case studies in the development of oil fields, design and operational data of industrial processes, performances of commercial products and others
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