当前位置: X-MOL 学术Environ. Chem. Lett. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Enhanced carbon resistance and regenerability in methane partial oxidation to syngas using oxygen vacancy-rich fibrous Pd, Ru and Rh/KCC-1 catalysts
Environmental Chemistry Letters ( IF 15.7 ) Pub Date : 2021-02-09 , DOI: 10.1007/s10311-021-01192-0
Tan Ji Siang , Aishah Abdul Jalil , Abdulrasheed Abdulrahman , Hambali Umar Hambali

Rising concerns about petroleum depletion and energy demand are calling for alternative processes such as methane partial oxidation to produce syngas for downstream synthetic fuel production. However, industrial application is limited by catalyst deactivation caused by carbon deposition and reoxidation of active metals. Here we synthesized dendritic fibrous Pd, Ru and Rh/KAUST Catalysis Centre 1 (KCC-1) catalysts by microemulsion followed by wetness impregnation. Catalysts were characterized by X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, electronic spin resonance, Fourier transform infrared spectroscopy and UV–Vis diffuse reflectance spectroscopy. We measured catalytic performance, stability and regenerability at 900 °C over 16 h-on-stream. Results reveal that oxygen vacancies into the KCC-1 framework enhance the interaction with noble metal particles, creating a strong metal–support interaction decreasing in the order Rh/KCC-1, Pd/KCC-1, Ru/KCC-1. Interestingly, CH4 conversion followed the same order: 74−80% for Rh/KCC-1, 60−71% for Pd/KCC-1, 53−63% for Ru/KCC-1, without a significant carbon deposit. These findings mean that oxygen vacancies retained the metal in the active metallic phase and prevented carbon deposits. Overall, metal/KCC-1 is as bifunctional catalyst whereby oxygen vacancies generate labile electrons contributing to electrostatic metal–support interactions, stabilization of metal phases and providing labile oxygen ions for carbon gasification.



中文翻译:

使用富氧空位的纤维状Pd,Ru和Rh / KCC-1催化剂,提高甲烷部分氧化成合成气的碳抗性和可再生性

对石油枯竭和能源需求的日益关注,要求采用替代工艺,例如甲烷部分氧化以生产用于下游合成燃料生产的合成气。然而,工业应用受到由碳沉积和活性金属再氧化引起的催化剂失活的限制。在这里,我们通过微乳液然后湿法浸渍合成了树枝状纤维状Pd,Ru和Rh / KAUST催化中心1(KCC-1)催化剂。通过X射线衍射,场发射扫描电子显微镜,透射电子显微镜,电子自旋共振,傅立叶变换红外光谱和UV-Vis漫反射光谱对催化剂进行了表征。我们在16小时的运转中900摄氏度下测量了催化性能,稳定性和可再生性。结果表明,进入KCC-1骨架的氧空位增强了与贵金属颗粒的相互作用,从而形成了强金属-载体相互作用,顺序降低了Rh / KCC-1,Pd / KCC-1,Ru / KCC-1。有趣的是,CH4次转化遵循相同的顺序:Rh / KCC-1为74-80%,Pd / KCC-1为60-71%,Ru / KCC-1为53-63%,且无大量碳沉积。这些发现意味着氧空位将金属保留在活性金属相中并防止了碳沉积。总体而言,金属/ KCC-1是一种双功能催化剂,氧空位产生不稳定的电子,从而促进静电金属载体相互作用,金属相的稳定并为碳气化提供不稳定的氧离子。

更新日期:2021-02-09
down
wechat
bug