甲烷化
钴
催化作用
水煤气变换反应
纳米颗粒
背景(考古学)
费托法
合成气
材料科学
粒径
化学工程
金属有机化学
粒子(生态学)
选择性
纳米技术
化学
有机化学
冶金
古生物学
海洋学
地质学
工程类
生物
作者
Xiao‐Yu Zhou,Gregory A. Price,Glenn J. Sunley,Christophe Copéret
标识
DOI:10.1002/anie.202314274
摘要
Cobalt-based catalysts are well-known to convert syngas into a variety of Fischer-Tropsch (FTS) products depending on the various reaction parameters, in particular particle size. In contrast, the reactivity of these particles has been much less investigated in the context of CO2 hydrogenation. In that context, Surface organometallic chemistry (SOMC) was employed to synthesize highly dispersed cobalt nanoparticles (Co-NPs) with particle sizes ranging from 1.6 to 3.0 nm. These SOMC-derived Co-NPs display significantly different catalytic performances under CO2 hydrogenation conditions: while the smallest cobalt nanoparticles (1.6 nm) catalyze mainly the reverse water-gas shift (rWGS) reaction, the larger nanoparticles (2.1-3.0 nm) favor the expected methanation activity. Operando X-ray absorption spectroscopy shows that the smaller cobalt particles are fully oxidized under CO2 hydrogenation conditions, while the larger ones remain mostly metallic, paralleling the observed difference of catalytic performances. This fundamental shift of selectivity, away from methanation to reverse water-gas shift for the smaller nanoparticles is noteworthy and correlates with the formation of CoO under CO2 hydrogenation conditions.
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