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Gas-Phase Synthesis of Ni–CeOx Hybrid Nanoparticles and Their Synergistic Catalysis for Simultaneous Reforming of Methane and Carbon Dioxide to Syngas
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-05-09 00:00:00 , DOI: 10.1021/acs.jpcc.8b00665
Teng-Yun Liang,Chih-Yuan Lin,Fang-Chun Chou,Meiqi Wang,De-Hao Tsai

We develop a new Ni–CeOx hybrid nanoparticle as a high-performance catalyst for dry reforming of methane with carbon dioxide (DRM) using a facile gas-phase synthetic approach. The crystallites of Ni and CeO2 were homogeneously self-assembled as a hybrid nanostructure, creating a large amount of Ni–Ce–O interface for a strong metal–support interfacial interaction. Chemical composition and oxidation state of the hybrid nanostructure were tunable directly in the aerosol state. The results show that the starting temperature of catalysis by Ni-based catalysts reduced by ∼150 °C through the hybridization with CeO2 followed by a direct H2 reduction in the aerosol state. In comparison to Ni-only nanoparticle, the Ni–CeOx hybrid nanoparticle showed stable and high conversion for CH4 and CO2 with a remarkably turnover frequency at low temperature (0.1 s–1 at 450 °C). The amount of coke formation greatly reduced by 18×, whereas the H2/CO ratio was constant at ∼0.8 by a 1.5× of the increase of CO2/CH4 ratio. The work demonstrated a facile route for controlled synthesis of Ni–CeOx hybrid nanoparticles with a very high catalytic activity and stability of DRM. The findings of this study can shed light on the mechanism of Ni–Ce–O synergistic catalysis, which can be especially useful for methane-based energy applications.

中文翻译:

Ni-CeO x杂化纳米颗粒的气相合成及其协同催化甲烷和二氧化碳同时重整为合成气

我们开发了一种新型的Ni-CeO x杂化纳米颗粒,作为一种高效的催化剂,可通过一种简便的气相合成方法将其与二氧化碳(DRM)一起用于甲烷的干法重整。Ni和CeO 2的晶体均质地自组装为杂化纳米结构,从而产生了大量的Ni-Ce-O界面,从而实现了强大的金属-载体界面相互作用。杂化纳米结构的化学组成和氧化态可直接在气溶胶状态下调节。结果表明,通过与CeO 2的杂交,Ni基催化剂的催化起始温度降低了约150°C,然后气溶胶态直接还原了H 2。与仅含镍的纳米粒子相比,Ni–CeO x杂化纳米粒子对CH 4和CO 2表现出稳定且高的转化率,并且在低温下(450 ° C时为0.1 s –1)具有明显的转换频率。焦炭的形成量大大减少了18倍,而H 2 / CO的比率由于CO 2 / CH 4的比率增加了1.5倍而恒定在〜0.8左右。这项工作证明了具有很高的催化活性和DRM稳定性的Ni-CeO x杂化纳米颗粒的受控合成的简便途径。这项研究的发现可以阐明Ni-Ce-O协同催化的机理,这对于基于甲烷的能源应用特别有用。
更新日期:2018-05-09
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