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Clay-Supported Molybdenum-Based Catalysts for Higher Alcohol Synthesis from Syngas
Gai-mei Wu1, Ji-long Zhou2, Mei-mei Lv2, Wei Xie2, Song Sun2, Chen Gao2, Wen-dong Wang*1, Jun Bao*2
1.Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China;2.National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
Abstract:
A kind of clay-supported K-Co-Mo catalyst was prepared by a sol-gel method combined with incipient wetness impregnation. The catalyst structure was characterized by X-ray diffraction, N2 adsorption-desorption, H2 temperature-programmed reduction, and X-ray photoelectron spectroscopy techniques and its catalytic performance for higher alcohol syn-thesis from syngas was investigated. The active components has a high dispersion on the clay support surface. The increase of the Mo loading promoted reduction of M6+ but had no signi cant in fluence on the reduction of Mo4+ and Co2+ species. After reduction, a kind of lower state Moδ+ (1<δ<4) species was observed on the surface. Compared with the unsupported catalyst, the clay supported K-Co-Mo catalysts showed much higher catalytic performance for alcohol formation. The reason can be explained that the supported catalyst have a high active surface area and the mesoporous structure prolonged the residence time of intermediates for alcohol formation to some extent, which promoted the formation of higher alcohols. The high activity of the catalyst reduced at 773 K may be attributed to the high content of Moδ+ (1<δ<4) species on the surface, which was regarded as the active site for the adsorption of nondissociative CO and responsible for the alcohol formation.
Key words:  Higher alcohol synthesis, Clay support, K-Co-Mo catalyst, Syngas
FundProject:
粘土担载的钼基催化剂的制备、结构及CO加氢合成醇性能
武改美1, 周纪龙2, 吕梅梅2, 谢威2, 孙松2, 高琛2, 汪文栋*1, 鲍骏*2
1.中国科学技术大学化学物理系,合肥230026;2.中国科学技术大学国家同步辐射实验室,合肥230029
摘要:
采用溶胶凝胶法与等体积浸渍相结合制备了一系列以粘土为载体的K-Co-Mo催化剂. 采用XRD、N2等温吸脱附、H26+的还原,但对Mo4+和Co2+的还原没有明显的影响. 催化剂经还原后,在其表面生成了一种更低价态的Moδ+(1<δ<4)物种,被认为是合成醇的活性中心. 与非负载催化剂相比,粘土担载的K-Co-Mo具有更高的合成醇性能. 负载型催化剂具有较高的活性物种分散度,并且其介孔结构在一定程度上延长了合成醇反应中间体的滞留时间,从而促进了低碳醇的生成. 经773 K还原的催化剂具有较高的活性,其原因可为催化剂表面具有较高含量的Moδ+物种.
关键词:  低碳醇合成,粘土载体,K-Co-Mo催化剂,合成气
DOI:10.1063/1674-0068/28/cjcp1504075
分类号: