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Re-promoted Ni-Mn bifunctional catalysts prepared by microwave heating for partial methanation coupling with water gas shift under low H2/CO conditions
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2017-12-29 , DOI: 10.1016/j.apcata.2017.12.026
Xinxin Dong , Baosheng Jin , Yiqing Sun , Kun Shi , Lei Yu

Re-promoted Ni-Mn bifunctional catalysts were prepared by microwave and conventional heating separately, and tested for partial methanation coupling with water gas shift (WGS) of simulated biomass gas in a fixed bed reactor. A series of characterization techniques including N2 isothermal adsorption, XRD, H2-TPR, H2-TPD, SEM, TEM and XPS were employed to examine the physico-chemical properties of the catalysts. With the reaction condition of 350 °C, H2/CO = 0.8 and H2O/CO = 1, 82.6% CO conversion, 70.0% CH4 selectivity and 82.8% CO2 growth rate were obtained on the Ni-Mn/Re-Al2O3 (MV) catalyst, which indicated its excellent synergetic effect on partial methanation coupling with WGS. According to the characterization results, it was found that microwave heating was beneficial to increase the dispersion of Ni species in comparison with conventional heating and the addition of Re promoter elevated the catalytic performance from both structural and electronic aspects, which was proven by the lowered reduction temperature of β-type NiO and the intensified electron cloud density of active Ni atoms, respectively. In addition, the sequence of Re impregnation also had impact on the catalytic performance. Step impregnation prepared Ni-Mn/Re-Al2O3 (MV) exhibited larger turnover frequency (TOF) than co-impregnation prepared Ni-Mn-Re/Al2O3 (MV) in the H2/CO range of 0.6–1.0, owing to the larger electron cloud density and better anti-coking ability of the former catalyst. The 110-h lifetime test further demonstrated the potential of stable Ni-Mn/Re-Al2O3 (MV) catalyst in industrial application.



中文翻译:

通过微波加热在低H 2 / CO条件下进行部分甲烷化与水煤气变换制得的重促进Ni-Mn双功能催化剂

通过微波和常规加热分别制备重促进的Ni-Mn双功能催化剂,并在固定床反应器中通过模拟生物质气体的水煤气变换(WGS)进行部分甲烷化偶联反应的测试。采用了一系列表征技术,包括N 2等温吸附,XRD,H 2 -TPR,H 2 -TPD,SEM,TEM和XPS,研究了催化剂的理化性质。在350°C,H 2 / CO = 0.8且H 2 O / CO = 1的反应条件下,在Ni-Mn / Re上获得了82.6%的CO转化率,70.0%的CH 4选择性和82.8%的CO 2生长速率。 -铝2 O 3(MV)催化剂,表明其与WGS部分甲烷化偶联具有出色的协同作用。根据表征结果,发现与常规加热相比,微波加热有利于增加Ni的分散性,并且添加Re促进剂从结构和电子方面都提高了催化性能,这通过降低还原来证明。 β型NiO的温度和活性Ni原子的增强电子云密度。另外,Re浸渍的顺序也对催化性能有影响。分步浸渍制备的Ni-Mn / Re-Al 2 O 3(MV)比共浸渍制备的Ni-Mn-Re / Al 2 O表现出更大的周转频率(TOF)。H 2 / CO范围在0.6-1.0之间的3(MV),由于前者催化剂具有更大的电子云密度和更好的抗焦化能力。110小时的寿命测试进一步证明了稳定的Ni-Mn / Re-Al 2 O 3(MV)催化剂在工业应用中的潜力。

更新日期:2017-12-29
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