Synergistic Pt-Co-Co2C multifunctional active sites for enhanced higher alcohol synthesis from syngas
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作者
Shen, Huachen; Liu, Kaidi; Zhang, Ranqing; Chen, Hanqing; Zhang, Peipei; Li, Sixuan; Zhao, Yonghui; Lin, Tiejun; Zhong, Liangshu
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刊物名称
CHEMICAL ENGINEERING JOURNAL
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年、卷、文献号
2025, ,
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关键词
Shen, Huachen; Liu, Kaidi; Zhang, Ranqing; Chen, Hanqing; Zhang, Peipei; Li, Sixuan; Zhao, Yonghui; Lin, Tiejun; Zhong, Liangshu
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摘要
Higher alcohol synthesis (HAS) from syngas is of great significance but remains challenging due to low activity, poor oxygenate selectivity, and low yields. Herein, a Pt-doped CoMn-based catalyst was developed to regulate CO activation and balance the dissociative and non-dissociative adsorption of CO, which favors oxygenate formation. Over the 1.23Pt-CoMn catalyst, a CO conversion of 49.9 % and a higher alcohol (HA) selectivity of 44.9 % were attained while a 2.2-fold enhancement in the space-time yield (STY) of higher alcohols was obtained on Pt-decorated CoMn catalyst compared to that of the Pt-free CoMn catalyst. Various characterization studies demonstrate that the presence of highly dispersed Pt delta+ sites around the Co center can provide an additional site for the non-dissociative adsorption of CO and form Pt-Co-Co2C multifunctional active sites which significantly increase the surface coverage of non-dissociative CO* species. Combined with the DFT results, it is further confirmed that the tricomponent synergy among Pt, Co0 and Co2C can substantially enhance the CO non-dissociative activation capability and significantly reduce the energy barrier for the coupling of CO*- containing species with alkyl species to form oxygenated products at the interfacial sites.