Yasuda Shuhei, Osuga Ryota, Kunitake Yusuke, Kato Kazuya, Fukuoka Atsushi, Kobayashi Hirokazu, Gao Min, Hasegawa Jun-Ya, Manabe Ryo, Shima Hisashi, Tsutsuminai Susumu, Yokoi Toshiyuki
Institute of Innovative Research, Tokyo Institute of Technology, 4259 Nagatsuta, Midori-ku, Yokohama, 226-8503, Japan.
Institute for Catalysis, Hokkaido University, Kita 21 Nishi 10, Kita-ku, Sapporo, 001-0021, Japan.
Commun Chem. 2020 Sep 16;3(1):129. doi: 10.1038/s42004-020-00375-0.
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 H/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 CH. 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.
开发在低温下将甲烷选择性氧化为合成气方面具有高性能的简单催化剂已引起广泛关注。在此，我们报道一种通过简便浸渍法合成的用于甲烷氧化的镍基固体催化剂。在MOR型沸石上成功形成了尺寸为1.6纳米的高度分散的超小NiO颗粒。该沸石负载的镍催化剂在973K下能持续实现97 - 98%的甲烷转化率、91 - 92%的CO产率（H/CO比为2.0），并且具有高耐久性，催化剂上没有严重的积碳现象。密度泛函理论计算证明了NiO粒径对CH的C - H解离过程的影响。NiO粒径的减小增强了源自NiO纳米颗粒的氧的产生，这有助于在还原环境下甲烷的氧化，有效生成合成气。
