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CO_2 methanation over Co-Ni bimetal-doped ordered mesoporous Al_2O_3 catalysts with enhanced low-temperature activities

机译:Co-Ni双金属掺杂有序介孔Al_2O_3催化剂上CO_2甲烷化的低温活性增强

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The Ni based catalysts have been considered as potential candidates for the CO2 methanation owing to the low cost. However, the poor low-temperature catalytic activities limit their large-scale industrial application. In order to address this challenge, a series of Co-Ni bimetal doped ordered mesoporous Al2O3 materials have been designed and fabricated via the one-pot evaporation induced self-assembly strategy and employed as the catalysts for CO2 methanation. It is found that the large specific surface areas (up to 260.0 m(2/)g), big pore volumes (up to 0.59 cm(3)/g), and narrow pore size distributions of these catalysts have been successfully retained after 700 degrees C calcination. The Co and Ni species are homogenously distributed among the Al2O3 matrix due to the unique advantage of the one-pot synthesis strategy. The strong interaction between metal and mesoporous framework have been formed and the severely thermal sintering of the metallic Co-Ni active centers can be successfully inhibited during the processes of catalyst reduction and 50 h CO2 methanation reaction. More importantly, the synergistic effect between Co and Ni can greatly enhance the low-temperature catalytic activity by coordinating the activation of H-2 and CO2, prominently decreasing the activation energy toward CO2 methanation. As a result, their low-temperature activities are evidently promoted. Furthermore, the effect of the Co/(Co + Ni) molar percentage ratio on the catalytic property has been also systematically investigated over these catalysts. It is found that only the catalyst with appropriate ratio (20.0%) behaves the optimum catalytic performances. Therefore, the current Co-Ni based ordered mesoporous materials promise potential catalysts for CO2 methanation. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
机译:由于低成本,Ni基催化剂被认为是CO 2甲烷化的潜在候选者。然而,不良的低温催化活性限制了它们的大规模工业应用。为了解决这一挑战,已经通过一锅蒸发诱导自组装策略设计和制造了一系列Co-Ni双金属掺杂的有序介孔Al2O3材料,并将其用作CO2甲烷化的催化剂。已发现,这些催化剂的比表面积大(高达260.0 m(2 /)g),大孔体积(高达0.59 cm(3)/ g)和狭窄的孔径分布已在700次后成功保留下来。 ℃煅烧。由于一锅合成策略的独特优势,Co和Ni物种均匀分布在Al2O3基体中。在催化剂还原和50 h CO2甲烷化反应过程中,金属与介孔骨架之间形成了牢固的相互作用,可以成功地抑制金属Co-Ni活性中心的严重热烧结。更重要的是,Co和Ni的协同作用可以通过协调H-2和CO2的活化作用大大增强低温催化活性,从而显着降低了向CO2甲烷化的活化能。结果,显然促进了它们的低温活性。此外,还已经在这些催化剂上系统地研究了Co /(Co + Ni)摩尔百分比比对催化性能的影响。发现只有具有适当比例(20.0%)的催化剂表现出最佳的催化性能。因此,当前的基于Co-Ni的有序介孔材料有望成为CO2甲烷化的潜在催化剂。 (C)2018氢能出版物有限公司。由Elsevier Ltd.出版。保留所有权利。

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