Yangyang Xie,Yingying Zhang,Honglei Fan,Jiahao Zhang,Qinglan Hao,Baojuan Dou,Xin Hu,Botao Teng
Adsorption is a promising strategy to remove harmful substances from Fischer-Tropsch synthesis (FTS) wastewater, and clarifying the adsorption mechanism is an important issue. In this paper, carbon nanotubes (CNTs) with different pore size were used for the adsorption of low-carbon alcohols (methanol, ethanol, propanol , butanol , pentanol) and acids (acetic acid, propanoic acid , butyric acid). After the micropores being occupied by chloroform , the percentage of micropores decrease is found to exhibit a positive correlation with adsorption capacity, indicating that the micropores dominanate the adsorption properties of alcohols and acids. Based on density functional theory (DFT) calculation results, the adsorption energy of pentanol is the largest and that of methanol is the smallest, in consistent with the experimental results. The similar polarity of pentanol with CNTs improves the adsorption property. Furthermore, with similar polarity, the kinetic diameter of adsorbate being close to the pore size is beneficial for improving adsorption behavior of CNTs.
High efficient production of lower alcohols (C 1 –C 5 mixed alcohols) from hydrogen rich bio-oil derived syngas was achieved in this work. A non-catalytic partial oxidation (NPOX) gasification technology was successfully applied in the production and conditioning of bio-oil derived syngas using bio-oil (BO) and emulsifying waste engine oil (EWEO) as feedstock . The effects of water addition and feedstock composition on the gasification performances were investigated. When the BO 20 and EWEO 30 was mixed with mass ratio of 1: 0.33, the maximum hydrogen yield of 93.7% with carbon conversion of 96.7% was obtained, and the hydrogen rich bio-oil derived syngas was effectively produced. Furthermore, a two-stage bed reactor was applied in the downstream process of lower alcohols synthesis from hydrogen rich bio-oil derived syngas (H 2 /CO/CO 2 /CH 4 /N 2 = 52.2/19.5/3.0/9.4/15.9, v/v). The highest carbon conversion of 42.5% and the maximum alcohol yield of 0.18 kg/kg cat h with selectivity of 53.8 wt% were obtained over the Cu/ZnO/Al 2 O 3 (2.5)//Cu 25 Fe 22 Co 3 K 3 /SiO 2 (2.5) catalyst combination system. The mechanism and evaluation for lower alcohols synthesis from model bio-oil derived syngas and model mixture gas were also discussed. The integrative process of hydrogen rich bio-oil derived syngas production and downstream lower alcohols synthesis, potentially providing a promising route for the conversion of organic wastes into high performance fuels and high value-added chemicals.
Catalytic reactions play a central role in chemical production, wherein the strength of the catalyst support is key to long-term stable operation. Simple and efficient strength enhancement methods for heterogeneous catalysis have received significant attention. Herein, we developed a variable-temperature gradient elution technology for low-carbon alcohols to improve the crushing strength of microspheres prepared using the sol–gel method in a microfluidic system. Based on gel fiber growth and rearrangement utilizing the hydrogen-bonding effect between low-carbon alcohols and pseudo-boehmite, the pore structure and fiber network can be reconstructed. Low-carbon alcohols with strong hydrogen bonds and low steric hindrance are more conducive to the formation of short fibers when constructing a dense gel network coordinated with higher alcohols. By combining long and short fiber cross-linked networks, the crushing strength of microspheres is significantly improved, and a dense pore structure with a small pore volume forms. After gradient elution, a crushing strength of up to 71.78 N/mm 2 can be achieved with a high specific surface area of 254.27 m 2 /g, which significantly exceeds that of commercial alumina supports with the same pore volume. This efficient method provides an important solution for the long-term, stable operation of catalysts.
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