Ayub Nur Athirah, Bahruji Hasliza, Mahadi Abdul Hanif
Centre of Advanced Material and Energy Sciences, Universiti Brunei Darussalam Jalan Tungku Link BE 1410 Brunei Darussalam
RSC Adv. 2021 Sep 27;11(50):31807-31816. doi: 10.1039/d1ra04115k. eCollection 2021 Sep 21.
Low temperature CO methanation is a favorable pathway to achieve high selectivity to methane while increasing the stability of the catalysts. A Ba promoted Ni/SmO catalyst was investigated for CO methanation at atmospheric pressure with the temperature ranging from 200-450 °C. 5Ni-5Ba/SmO showed significant enhancement of CO conversion particularly at temperatures ≤ 300 °C compared to Ni/SmO. Incorporation of Ba into 5Ni/SmO improved the basicity of the catalysts and transformed the morphology of SmO from random structure into uniform groundnut shape nanoparticles. The uniformity of SmO created interparticle porosity that may be responsible for efficient heat transfer during a long catalytic reaction. Ba is also postulated to catalyze oxygen vacancy formation on SmO under a reducing environment presumably isomorphic substitution. The disappearance of a high temperature (∼600 °C) reduction peak in H-TPR analysis revealed the reducibility of NiO following impregnation with Ba. However, further increasing the Ba loading to 15% formed BaNiO-BaNiO phases which consequently reduced the activity of the Ni-Ba/SmO catalyst at low temperature. Ni was suggested to segregate from BaNiO-BaNiO at high temperature thus exhibiting comparable activity with Ni/SmO at 450 °C.
低温CO甲烷化是一种在提高催化剂稳定性的同时实现对甲烷高选择性的有利途径。研究了一种Ba促进的Ni/SmO催化剂在大气压下、200 - 450℃温度范围内的CO甲烷化反应。与Ni/SmO相比,5Ni-5Ba/SmO在温度≤300℃时CO转化率有显著提高。向5Ni/SmO中引入Ba提高了催化剂的碱性,并将SmO的形态从无规则结构转变为均匀的花生状纳米颗粒。SmO的均匀性产生了颗粒间孔隙,这可能是长催化反应过程中有效传热的原因。据推测,在还原环境下,Ba可能通过同晶取代催化SmO上氧空位的形成。H-TPR分析中高温(~600℃)还原峰的消失表明用Ba浸渍后NiO的可还原性。然而,将Ba负载量进一步提高到15%会形成BaNiO-BaNiO相,从而降低了Ni-Ba/SmO催化剂在低温下的活性。有人认为Ni在高温下会从BaNiO-BaNiO中分离出来,因此在450℃时表现出与Ni/SmO相当的活性。