Hierarchical leaf-like alumina-carbon nanosheets with ammonia water modification for ethanol dehydration to ethylene

纳米片 催化作用 脱水 选择性 乙烯 化学 脱水反应 无机化学 乙醇 化学工程 材料科学 有机化学 生物化学 工程类
作者
Yan Hao,Dajie Zhao,Yang Zhou,Maorui Yin,Zhiqiang Wang,Guoxi Xi,Shili Song,Qinghu Tang,Jinghe Yang
出处
期刊:Fuel [Elsevier BV]
卷期号:333: 126128-126128 被引量:19
标识
DOI:10.1016/j.fuel.2022.126128
摘要

• Alumina-carbon catalysts have leaf-like nanosheet structures and Brönsted acid active sites. • The catalyst exhibits a remarkably high TOF of 361.8 h −1 and ethylene selectivity of 97 %. • The catalyst maintains a good stability upon time on stream of 144 h at 450 ℃. A hierarchical leaf-like alumina-carbon nanosheet catalyst was prepared by a chelate-assisted co-assembly method to improve the catalytic behavior of ethanol dehydration reaction, based on the chemical etching effect of ammonia water. The uniformly dispersed leaf-like nanosheet structure possessed a relatively large specific surface area and exposed more active sites, which could promote the ethanol dehydration reaction. This catalyst was promising to obtain a higher catalytic behavior (conversion of 98.3 % and ethylene selectivity of 97.0 %) than the sample without ammonia water modification (conversion of 63.2 % and ethylene selectivity of 46.7 %) at 450 ℃. The addition of ammonia water played an essential role in influencing the formation of the leaf-like nanosheet structure and the generation of Brönsted acid active sites, which remarkably promoted the proceed of ethanol dehydration. Importantly, a direct relationship was observed between the nanosheet thickness and the alumina content. The best catalytic activity with TOF of 361.8 h −1 was obtained when the Al loading of 13.9 wt%, attributed to the suitably balanced weak/moderate acidic active sites ratio of ∼ 4.37. In-situ FTIR spectra of ethanol dehydration reaction clearly confirmed that ethanol was first converted to the intermediate product diethyl ether and then subsequently decomposed to ethylene at a higher temperature. The catalyst also maintained a good recyclability upon time on stream of 144 h at 450 ℃. This work provides an alternative way of developing non-noble metal catalyzing ethanol dehydration to ethylene.
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