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Adjusted interactions of nickel nanoparticles with cobalt-modified MgAl2O4-SiC for an enhanced catalytic stability during steam reforming of propane
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2017-09-28 , DOI: 10.1016/j.apcata.2017.09.031
Kyung Soo Park , Minji Son , Myung-June Park , Dae Hyun Kim , Jeong Hwa Kim , So Hyun Park , Joon-Hwan Choi , Jong Wook Bae

Steam reforming of propane (SRP) for the stable production of hydrogen-rich reformates was investigated using the Ni-supported on the cobalt-modified SiC-embedded MgAl2O4 support (denoted as NCMAS). The adjusted interactions of the Ni nanoparticles with the cobalt-modified SiC-embedded MgAl2O4 (MgAl2O4-SiC) and its crystallite size distributions largely altered the catalytic activity and stability of NCMAS. The introductions of SiC on the NCMAS, where SiC has a higher thermal conductivity, also increased the dispersion of smaller MgAl2O4 grains with the less formations of inactive NiAl2O4 species, which resulted in the higher catalytic activity with smaller formations of unreformed light hydrocarbons. The positive roles of cobalt promoter on the MgAl2O4-SiC matrices were mainly attributed to the suppressed aggregation of nickel nanoparticles by their strong and intimate interactions with the cobalt-modified MgAl2O4. The effects of cobalt promoter at an optimal 5wt%Co in the MgAl2O4-SiC (NCMAS(5)) enhanced the oxidation-resistance of the nickel nanoparticles with less formations of inactive metal aluminates by being reversibly re-reduced under the SRP reaction conditions. These phenomena further lessen coke depositions by intimately interacting with highly dispersed oxophilic cobalt or cobalt aluminate species. The optimal NCMAS(5) was applied to derive kinetic parameters using Langmuir-Hinshelwood-Hougen-Watson (LHHW) mechanisms, and the reasonable activation energy of 73 kJ/mol and optimal operating parameters to maximize hydrogen production by SRP reaction was estimated in terms of the reaction conditions such as space velocity, feed ratio and reaction temperature.



中文翻译:

镍纳米颗粒与钴改性的MgAl 2 O 4 -SiC的调节相互作用,以提高丙烷蒸汽重整过程中的催化稳定性

使用钴改性的SiC嵌入的MgAl 2 O 4载体(表示为NCMAS)上的镍负载,研究了丙烷的蒸汽重整(SRP)以稳定生产富氢重整产品。Ni纳米粒子与钴改性的SiC嵌入的MgAl 2 O 4(MgAl 2 O 4 -SiC)的调节相互作用及其微晶尺寸分布大大改变了NCMAS的催化活性和稳定性。在NCMAS上引入SiC时,SiC具有较高的导热性,这也增加了较小的MgAl 2 O 4晶粒的分散性,并且减少了惰性NiAl 2 O 4的形成。物种,从而导致较高的催化活性,并形成较少量的未重整轻烃。钴促进剂在MgAl 2 O 4 -SiC基质上的积极作用主要归因于其与钴改性的MgAl 2 O 4的强而密切的相互作用,从而抑制了镍纳米粒子的聚集。MgAl 2 O 4中最佳钴含量为5wt%时钴助催化剂的作用-SiC(NCMAS(5))通过在SRP反应条件下可逆还原,可减少具有较少惰性金属铝酸盐形成的镍纳米粒子的抗氧化性。这些现象通过与高度分散的嗜氧钴或铝酸钴物种密切相互作用而进一步减少了焦炭沉积。利用Langmuir-Hinshelwood-Hougen-Watson(LHHW)机理应用了最佳NCMAS(5)得出动力学参数,并估算了合理的活化能73 kJ / mol和最佳操作参数,以通过SRP反应最大程度地产氢。反应条件如空速,进料比和反应温度。

更新日期:2017-09-28
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