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Zeolite-supported ultra-small nickel as catalyst for selective oxidation of methane to syngas
Communications Chemistry ( IF 5.9 ) Pub Date : 2020-09-16 , DOI: 10.1038/s42004-020-00375-0
Shuhei Yasuda 1 , Ryota Osuga 1 , Yusuke Kunitake 1 , Kazuya Kato 2 , Atsushi Fukuoka 2 , Hirokazu Kobayashi 2 , Min Gao 2 , Jun-Ya Hasegawa 2 , Ryo Manabe 3 , Hisashi Shima 3 , Susumu Tsutsuminai 3 , Toshiyuki Yokoi 1
Affiliation  

The development of simple catalysts with high performance in the selective oxidation of methane to syngas at low temperature has attracted much attention. Here we report a nickel-based solid catalyst for the oxidation of methane, synthesised by a facile impregnation method. Highly dispersed ultra-small NiO particles of 1.6 nm in size are successfully formed on the MOR-type zeolite. The zeolite–supported nickel catalyst gives continuously 97–98% methane conversion, 91–92% of CO yield with a H2/CO ratio of 2.0, and high durability without serious carbon deposition onto the catalyst at 973 K. DFT calculations demonstrate the effect of NiO particle size on the C-H dissociation process of CH4. A decrease in the NiO particle size enhances the production of oxygen originating from the NiO nanoparticles, which contributes to the oxidation of methane under a reductive environment, effectively producing syngas.



中文翻译:

沸石负载超细镍催化剂用于甲烷选择性氧化制合成气

开发在甲烷低温选择性氧化制合成气中具有高性能的简单催化剂备受关注。在这里,我们报告了一种用于甲烷氧化的镍基固体催化剂,该催化剂通过简便的浸渍法合成。在 MOR 型沸石上成功形成了尺寸为 1.6 nm 的高度分散的超小 NiO 颗粒。沸石负载的镍催化剂连续提供 97–98% 的甲烷转化率、91–92% 的 CO 产率(H 2 /CO 比率为 2.0)和高耐久性,在 973 K 时催化剂上没有严重的碳沉积。DFT 计算表明NiO粒径对CH 4 CH解离过程的影响. NiO 颗粒尺寸的减小增强了源自 NiO 纳米颗粒的氧的产生,这有助于甲烷在还原环境下的氧化,有效地产生合成气。

更新日期:2020-09-16
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