Improved Selectivity of Long-Chain Products from Aqueous Acetone-Butanol-Ethanol Mixture over High Water Resistant Catalyst Based on Hydrophobic SBA-16
Improved Selectivity of Long-Chain Products from Aqueous Acetone-Butanol-Ethanol Mixture over High Water Resistant Catalyst Based on Hydrophobic SBA-16
复制标题
基于疏水性 SBA-16 的高耐水催化剂提高了丙酮-丁醇-乙醇水混合物中长链产物的选择性
DOI：
10.1021/acssuschemeng.9b00190
复制
发表时间：
2019
影响因子：
8.4
通讯作者：
Tan Tianwei
中科院分区：
文献类型：
--
作者：
Gong Yahui;Shen Chun;Wang Jie;Wu Cai;Tan Tianwei
在从发酵产物获得生物燃料的过程中，催化剂的耐水性和/或水热稳定性是关键问题，其总是涉及大量的水。本文针对含水丙酮-丁醇-乙醇（ABE）发酵混合物高效升级为长链产物的问题，设计并合成了一系列10 wt %的Ni-MgO-SBA-16催化剂，该催化剂以具有高度缩合结构的疏水性SBA-16为基础。这些催化剂具有较低的水吸附能力和较好的疏水性。在无溶剂条件下，C5- 15物种的转化率和选择性分别达到76.4%和90.5%;当初始水含量增加到7.4wt%时，C5 - 15物种的转化率和总选择性也达到了相当的水平。此外，由于疏水表面的存在，即使在高含水量的条件下，单烷基化产物也容易转化为双烷基化产物。结果表明，10 wt % Ni-MgO-SBA-16催化剂具有“一石二鸟”的作用：提高了催化剂的耐水性和水热稳定性，抑制了水分子的竞争吸附，促进了疏水中间体2-庚酮的吸附转化为长链烃;用贱金属代替稀有贵金属，符合“绿色化学”的原则。总之，本工作不仅在含水ABE的增值方面取得了重大进展，而且为生物质转化过程中需要高水热稳定性和/或耐水性的催化剂的合理合成方向提供了参考。
Water resistance and/or hydrothermal stability of catalysts are key concerns during the obtention of biofuels from fermentation products, which always involve considerable amounts of water. Herein, aimed at efficient upgrading of a water-containing acetone–butanol–ethanol (ABE) fermentation mixture to long-chain products, we designed and synthesized a series of 10 wt % Ni–MgO–SBA-16 catalysts, which were based on hydrophobic SBA-16 with highly condensed structures. These catalysts exhibited low water adsorptive capacities and relatively favorable hydrophobicity. As expected, the as-prepared catalysts showed excellent catalytic activity and water-tolerance: 76.4% conversion and 90.5% selectivity for C5–15species were achieved under solvent-free conditions; when the initial water content increased to 7.4 wt %, comparable conversion and total selectivity for C5–15species were also achieved. Besides, on account of the hydrophobic surface, monoalkylation products readily converted into doublealkylation ones even under conditions of high water content. The results demonstrated the 10 wt % Ni–MgO–SBA-16 catalysts acted as the role of “killing two birds with one stone”: promoting the water tolerance and exhibiting high hydrothermal stability; suppressing competitive adsorption of water molecules and facilitating the adsorption and transformation of hydrophobic intermediate 2-heptanone to long-chain hydrocarbons; replacing the rare noble metal by base metal and complying with the principles of “green chemistry”. Overall, this work not only makes significant progress in value-adding of water-containing ABE but also provides the rational synthetic direction of catalysts requiring high hydrothermal stability and/or water resistance in the biomass conversion process.