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Effect of Preparation Technique on the Performance of Ni and Ce Incorporated Modified Alumina Catalysts in CO2 Reforming of Methane
Catalysis Letters ( IF 2.8 ) Pub Date : 2020-04-25 , DOI: 10.1007/s10562-020-03228-6
Huseyin Arbag , H. Mehmet Tasdemir , Yavuz Yagizatli , Melike Kucuker , Sena Yasyerli

Performances of modified sol–gel alumina (MSGA) based catalysts, synthesized in an inert atmosphere and activated by Ni and Ce were investigated in CO2 reforming of methane. Two different incorporation methods were used to dope Ce into the structure of the catalysts: (i) simultaneous impregnation of Ce together with Ni (Ni–Ce@MSGA), (ii) one-pot synthesis of Ce incorporated alumina support material (Ni@Ce-MSGA). In the second case Ni was impregnated on the Ce-MSGA support. Synthesized catalysts were characterized using TPR, XRD, N2 adsorption/desorption, pyridine adsorbed DRIFT, CO2-TPD techniques. These analyses showed that the synthesized catalysts possessed reduced Ni particles, as well as mesoporous structure, Lewis acid sites and moderate basicity. The modified sol–gel alumina and modified sol–gel Ce-MSGA supported catalysts showed stable activity in CO2 reforming of methane. Ce incorporation improved catalytic activity of the synthesized catalysts and reduced the occurrence of reverse water gas shift reaction. Ni–Ce@MSGA catalyst decreased the CO2/CH4 conversion ratio much higher than Ni@Ce-MSGA catalyst. Coke analysis were determined using TGA/DTA, XRD, and SEM analysis. Especially, simultaneous impregnation of Ce and Ni catalyst inhibited coke deposition significantly due to lattice oxygen of ceria. However, coke deposition over Ni@Ce-MSGA catalyst was higher than Ni@MSGA catalyst since Ni@Ce-MSGA catalyst has higher nickel crystal size than that of Ni@MSGA catalyst.

中文翻译:

制备工艺对Ni、Ce改性氧化铝催化剂CO2甲烷重整性能的影响

研究了在惰性气氛中合成并由 Ni 和 Ce 活化的改性溶胶-凝胶氧化铝 (MSGA) 基催化剂在甲烷的 CO2 重整中的性能。使用两种不同的掺入方法将 Ce 掺杂到催化剂的结构中:(i)Ce 与 Ni(Ni–Ce@MSGA)同时浸渍,(ii)一锅法合成掺 Ce 的氧化铝载体材料(Ni@ Ce-MSGA)。在第二种情况下,镍浸渍在 Ce-MSGA 载体上。合成的催化剂使用 TPR、XRD、N2 吸附/解吸、吡啶吸附 DRIFT、CO2-TPD 技术进行表征。这些分析表明合成的催化剂具有还原的 Ni 颗粒、介孔结构、路易斯酸位点和中等碱性。改性溶胶-凝胶氧化铝和改性溶胶-凝胶 Ce-MSGA 负载的催化剂在甲烷的 CO2 重整中表现出稳定的活性。Ce的掺入提高了合成催化剂的催化活性并减少了逆水煤气变换反应的发生。Ni-Ce@MSGA 催化剂降低的 CO2/CH4 转化率远高于 Ni@Ce-MSGA 催化剂。使用 TGA/DTA、XRD 和 SEM 分析确定焦炭分析。特别是,由于氧化铈的晶格氧,Ce和Ni催化剂的同时浸渍显着抑制了焦炭沉积。然而,Ni@Ce-MSGA 催化剂上的焦炭沉积高于 Ni@MSGA 催化剂,因为 Ni@Ce-MSGA 催化剂具有比 Ni@MSGA 催化剂更大的镍晶体尺寸。Ce的掺入提高了合成催化剂的催化活性并减少了逆水煤气变换反应的发生。Ni-Ce@MSGA 催化剂降低的 CO2/CH4 转化率远高于 Ni@Ce-MSGA 催化剂。使用 TGA/DTA、XRD 和 SEM 分析确定焦炭分析。特别是,由于氧化铈的晶格氧,Ce和Ni催化剂的同时浸渍显着抑制了焦炭沉积。然而,Ni@Ce-MSGA 催化剂上的焦炭沉积高于 Ni@MSGA 催化剂,因为 Ni@Ce-MSGA 催化剂具有比 Ni@MSGA 催化剂更大的镍晶体尺寸。Ce的掺入提高了合成催化剂的催化活性并减少了逆水煤气变换反应的发生。Ni-Ce@MSGA 催化剂降低的 CO2/CH4 转化率远高于 Ni@Ce-MSGA 催化剂。使用 TGA/DTA、XRD 和 SEM 分析确定焦炭分析。特别是,由于氧化铈的晶格氧,Ce和Ni催化剂的同时浸渍显着抑制了焦炭沉积。然而,Ni@Ce-MSGA 催化剂上的焦炭沉积高于 Ni@MSGA 催化剂,因为 Ni@Ce-MSGA 催化剂具有比 Ni@MSGA 催化剂更大的镍晶体尺寸。由于氧化铈的晶格氧,Ce和Ni催化剂的同时浸渍显着抑制了焦炭沉积。然而,Ni@Ce-MSGA 催化剂上的焦炭沉积高于 Ni@MSGA 催化剂,因为 Ni@Ce-MSGA 催化剂具有比 Ni@MSGA 催化剂更大的镍晶体尺寸。由于氧化铈的晶格氧,Ce和Ni催化剂的同时浸渍显着抑制了焦炭沉积。然而,Ni@Ce-MSGA 催化剂上的焦炭沉积高于 Ni@MSGA 催化剂,因为 Ni@Ce-MSGA 催化剂具有比 Ni@MSGA 催化剂更大的镍晶体尺寸。
更新日期:2020-04-25
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