氧化铝制备工艺对银催化剂性能的影响
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摘要
研究了不同类型氧化铝晶体形貌与制备工艺对银催化剂及其载体性能的影响。结果表明,经高温焙烧后,氧化铝晶粒虽然已经有长大的趋势,但未完全发育,仍存在很多"蠕虫状"无规则氧化铝晶粒;其中,添加硼化物载体的晶粒长得相对更完整一些,对块状氧化铝的生成较为有利;添加胺基化合物有利于水合氧化铝向α-氧化铝的转变,但其实际效果稍低于硼化物。采用比表面积较高的氧化铝作为载体,制得的银催化剂的反应活性较高。若通过添加造孔剂形成较大气孔,催化剂的选择性得到明显提高。
The effects of different types of alumina crystal morphology and preparation process on the performances of silver catalyst and its support were studied.The results indicated that the alumina grains had a tendency to grow after calcinations at high temperature,but it was not fully developed,and there were still many"worm-like"irregular alumina grains.Meanwhile,the alumina grain with addition of boride was relatively more complete,which was more favorable for the formation of bulk alumina.Amine compound was beneficial to the conversion of hydrated alumina to α-alumina,but its actual effect was slightly lower than that of boride.The silver catalyst prepared by the carrier with a high specific surface area had high activity.If a large pore of carrier was formed by adding a pore former,the selectivity of the catalyst was remarkably improved.
The effects of different types of alumina crystal morphology and preparation process on the performances of silver catalyst and its support were studied.The results indicated that the alumina grains had a tendency to grow after calcinations at high temperature,but it was not fully developed,and there were still many"worm-like"irregular alumina grains.Meanwhile,the alumina grain with addition of boride was relatively more complete,which was more favorable for the formation of bulk alumina.Amine compound was beneficial to the conversion of hydrated alumina to α-alumina,but its actual effect was slightly lower than that of boride.The silver catalyst prepared by the carrier with a high specific surface area had high activity.If a large pore of carrier was formed by adding a pore former,the selectivity of the catalyst was remarkably improved.
引文
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[2]杨忠兵.环氧乙烷产业技术现状与展望[J].石油化工技术与经济,2014,30(6):52-56.
[3]孙果宋,李华锋,王俊,等.环氧乙烷深加工产品生产技术进展[J].精细化工,2010,27(10):937-941.
[4]赵楠楠.环氧乙烷生产技术进展及产能现状[J].化工时刊,2015,29(5):23-26.
[5]崔小明.环氧乙烷生产技术进展及市场分析[J].精细与专用化学品,2014,22(5):12-18.
[6]刘宗语.环氧乙烷/乙二醇生产技术进展[J].化工进展,2013,32(6):1214-1218.
[7]Suljo Linic,Mark A Barteau.Formation of a stable surface oxametallacycle that produces rthylene oxide[J].J Am Chem Soc,2002,124(2),310-317.
[8]Podgornov E A,Prosvirin I P,Bukhtiyarov V I.XPS,TPD and TPRstudies of Cs-O complexes on silver:Their role in ethylene epoxidation[J].Journal of Molecular Catalysis A:Chemical,2000,158(1):337-343.
[9]Stegelmann C,Schidt N C,Campbell C T,et al.Microkinetic modeling of ethylene oxidation over silver[J].Journal of Catalysis,2004,221(2):630-649.
[10]Piao H,Enever M C N,Adib K,et al.High resolution X-ray photoelectron spectroscopy of styrene oxide adsorption and reaction on Ag(111)[J].Surface Science,2004,571(1-3):139-145.
[11]Siriphong Rojluechai,Sumaeth Chavadej,Johannes W Schwank,et al.Activity of ethylene epoxidation over high surface area alumina support Au-Ag catalysts[J].Journal of Chemical Engineering of Japan,2006,39(3):321-326.
[12]Enever M,Linic S,Uffalussy K,et al.Synthesis,structure,and reactions of stable oxametallacycles from styrene oxide on Ag(111)[J].J Phys Chem B,2005,109(6):2227-2233.
[13]Suljo Linic,Mark A Barteau.Control of ethylene epoxidation selectivity by surface oxametallacycles[J].Journal of the American Chemical Society,2003,125(14):4034-4035.
[14]Lauritzen,Ann M.Ethylene oxide catalyst and process for preparing the catalyst:US,4761394[P].1988-08-02.
[15]Lauritzen,Ann M.Ethylene oxide catalyst and process for preparing the catalyst:US,4766105[P].1988-08-23.
[16]周允红,周晓龙,曹建春,等.负载银催化剂的制备与应用的研究进展[J].石油化工,2014,43(6):721-728.
[17]Nabil Rizkalla,Andrzej Rokicki.Carrier treatment to improve catalytic performance of an ethylene oxide catalyst:US,2017/0369460A1[P].2017-12-28.
[18]Dellamorte J C,Lauterbach J,Barteau M A.Promoter-induced morphological changes of Ag catalysts for ethylene epoxidation[J].Ind Eng Chem Res,2009,48(13):5943-5953.
[19]皇环环,王倩,吴丽,等.低温燃烧合成法制备的氧化铝陶瓷粉体的发光特性[J].光谱学与光谱分析,2018,38(9):2676-2680.
[20]刘峰,何德东,陆继长,等.尿素研磨燃烧法合成Ce0.8Zr0.2O2固溶体对乙硫醇催化分解的研究[J].中国稀土学报,2018,36(1):53-60.