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Co–Co2C catalysts supported on carbon-coated ordered mesoporous silica with promoted CO insertion and C–C coupling for higher alcohol synthesis from syngas
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2024-04-10 , DOI: 10.1039/d4ta01179a
Zhuoshi Li 1, 2 , Siqi Fan 1 , Zhuang Zeng 1 , Shaoxia Guo 1 , Xiaofeng Pei 1 , Shouying Huang 1, 3 , Yong Wang 1 , Yue Wang 1, 2, 3 , Xinbin Ma 1, 3
Affiliation  

Higher alcohol synthesis (HAS) from syngas is a potential energy conversion route which has attracted extensive interest from both academia and industry. Co–Co2C catalysts are promising candidates for HAS, but the yield of higher alcohols (HAs) and catalyst stability still need to be promoted. Here, a series of carbon-coated ordered mesoporous silica (OMS) supported cobalt catalysts were prepared with modulated carbon layer thicknesses. Co/10C/OMS with a carbon layer of 0.55 nm achieved an optimal ROH selectivity of 41.3%, space time yield (STY) towards a HA of 23.7 mmol gcat−1 h−1 and stability over 300 h. As the carbon layer thickened, particle dispersion was facilitated and the metal-support interaction was modulated, which resulted in the volcanic variation of the surface Co2C/Co0 ratio. In addition, compared to a carbon-coated amorphous SiO2 supported sample, significant CO enrichment was observed inside the ordered mesopores in Co/xC/OMS, which enhanced the CO insertion and C–C coupling, boosting the selectivity of HA. This work may give insights into the use of carbon–silica composite supports and the design of high-performance Co–Co2C catalysts for HAS.

中文翻译:

碳包覆有序介孔二氧化硅负载 Co-Co2C 催化剂,促进 CO 插入和 C-C 偶联,用于合成气合成高级醇

合成气合成高级醇(HAS)是一种潜在的能源转化途径,引起了学术界和工业界的广泛兴趣。 Co-Co 2 C催化剂是HAS的有希望的候选者,但高级醇(HA)的产率和催化剂稳定性仍需要提高。在此,制备了一系列具有调节碳层厚度的碳包覆有序介孔二氧化硅(OMS)负载钴催化剂。具有0.55 nm碳层的Co/10C/OMS实现了41.3%的最佳ROH选择性、23.7 mmol g cat -1 h -1的HA的时空产率(STY)和300小时以上的稳定性。随着碳层增厚,颗粒分散得到促进,金属-载体相互作用得到调节,导致表面Co 2 C/Co 0比值发生火山变化。此外,与碳包覆的无定形SiO 2负载样品相比,在Co/ x C/OMS的有序介孔内观察到显着的CO富集,这增强了CO插入和C-C耦合,提高了HA的选择性。这项工作可能有助于深入了解碳-二氧化硅复合载体的使用以及用于 HAS 的高性能 Co-Co 2 C 催化剂的设计。
更新日期:2024-04-10
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