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Nickel nanoparticles supported on nitrogen–doped carbon nanotubes are a highly active, selective and stable CO2 methanation catalyst
Journal of Energy Chemistry ( IF 14.0 ) Pub Date : 2020-06-17 , DOI: 10.1016/j.jechem.2020.06.007
Julian Gödde , Mariia Merko , Wei Xia , Martin Muhler

CO2 methanation using nickel-based catalysts has attracted large interest as a promising power-to-gas route. Ni nanoparticles supported on nitrogen-doped CNTs with Ni loadings in the range from 10 wt% to 50 wt% were synthesized by impregnation, calcination and reduction and characterized by elemental analysis, X-ray powder diffraction, H2 temperature-programmed reduction, CO pulse chemisorption and transmission electron microscopy. The Ni/NCNT catalysts were highly active in CO2 methanation at atmospheric pressure, reaching over 50% CO2 conversion and over 95% CH4 selectivity at 340 °C and a GHSV of 50,000 mL g−1 h−1 under kinetically controlled conditions. The small Ni particle sizes below 10 nm despite the high Ni loading is ascribed to the efficient anchoring on the N-doped CNTs. The optimum loading of 30 wt%–40 wt% Ni was found to result in the highest Ni surface area, the highest degree of conversion and the highest selectivity to methane. A constant TOF of 0.3 s−1 was obtained indicating similar catalytic properties of the Ni nanoparticles in the range from 10 wt% to 50 wt% Ni loading. Long-term experiments showed that the Ni/NCNT catalyst with 30 wt% Ni was highly stable for 100 h time on stream.



中文翻译:

氮掺杂碳纳米管上负载的镍纳米颗粒是高活性,选择性和稳定的CO 2甲烷化催化剂

使用镍基催化剂的CO 2甲烷化作为一种​​有前途的动力气路线引起了广泛的兴趣。通过浸渍,煅烧和还原合成了负载在10%(重量)至50%(重量)的掺氮CNT上的Ni纳米颗粒,并通过元素分析,X射线粉末衍射,H 2程序升温还原,CO脉冲化学吸附和透射电子显微镜。Ni / NCNT催化剂在大气压下在CO 2甲烷化中具有很高的活性,在340°C和GHSV为50,000 mL g -1  h -1的条件下,CO 2转化率超过50%,CH 4选择性超过95%。在动力学控制的条件下。尽管Ni含量较高,但10 nm以下的Ni颗粒较小,这归因于N掺杂CNT的有效锚固。发现最佳负载量为30 wt%–40 wt%Ni可导致最高的Ni表面积,最高的转化度和最高的甲烷选择性。获得0.3 s -1的恒定TOF,表明Ni纳米颗粒在10重量%至50重量%的镍负载量范围内具有相似的催化性能。长期实验表明,含30%(重量)Ni的Ni / NCNT催化剂在运行100小时内具有很高的稳定性。

更新日期:2020-06-17
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