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Chemically activated poly(furfuryl alcohol)-derived CMK-3 carbon catalysts for the oxidative dehydrogenation of ethylbenzene

机译:化学活化的聚糠醇衍生的CMK-3碳催化剂用于乙苯的氧化脱氢

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The surface of CMK-3 carbon, synthesized by the reversible replication of mesoporous silica (SBA-15) using poly(furfuryl alcohol) as a carbon precursor, was activated by wet oxidation with an aqueous solution of HNO3 or H2O2. The process was performed at 50 °C using solution containing different concentrations of the oxidizing agent. It was found that during the modification no significant changes in textural and structural properties of CMK-3 replica occurred. However, the treatment resulted in the formation of appreciable amounts of surface species containing oxygen. XPS and DRIFTspectroscopy allowed to identify and quantify the surface functional groups. Their stability was studied by TG-FTIR measurements. CO and CO2 were found as main gaseous products evolved during thermal decomposition under inert atmosphere. Finally, the modified samples were tested in the catalytic oxidative dehydrogenation of ethylbenzene to styrene at 350 °C in the presence of oxygen as an oxidizing agent (at O2/ethylbenzene molar ratio of 1.0 and 3.0). At the beginning of the catalytic run, the highest styrene yield and selectivity was achieved at the lower O2 content over the catalysts treated with nitric acid. Nevertheless, all studied catalysts underwent a gradual deactivation due to coke formation and changes in the distribution of surface moieties.
机译:通过使用HNO3或H2O2水溶液进行湿式氧化,活化通过使用聚乙烯醇作为碳前体的中孔二氧化硅(SBA-15)可逆复制而合成的CMK-3碳表面。使用含有不同浓度氧化剂的溶液在50°C下进行该过程。发现在修饰期间,CMK-3复制品的质地和结构性质没有显着变化。但是,该处理导​​致形成了相当数量的含氧表面物质。 XPS和DRIFT光谱法可以识别和定量表面官能团。通过TG-FTIR测量研究了它们的稳定性。发现CO和CO2是惰性气氛下热分解过程中释放出的主要气体产物。最后,在氧作为氧化剂存在下(O2 /乙苯摩尔比为1.0和3.0),在350°C下乙苯催化氧化脱氢为苯乙烯,测试了改性样品。在催化操作开始时,与用硝酸处理的催化剂相比,在较低的O2含量下,苯乙烯的收率和选择性最高。然而,由于焦炭的形成和表面部分分布的变化,所有研究的催化剂都逐渐失活。

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