Controlling the reaction network of Ni/silica derived conversion of bio-oil surrogate guaiacol

IF 6.4 3区环境科学与生态学 Q2 ENERGY & FUELS

Carbon Resources Conversion Pub Date : 2023-06-02 DOI:10.1016/j.crcon.2023.05.006

Nils Kretzschmar, Oliver Busse, Markus Seifert

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Abstract

Replacing fossil carbon sources with green bio-oils is a promising route to switch to a sustainable chemical industry, although their high oxygen contents are challenging. Catalytic hydrodeoxygenation is a favored route to upgrade bio-oils to renewable fuels and basic chemicals. In this work, we investigated Ni/SiO₂ catalysts with differing metal dispersity in continuous mode conversion of guaiacol with a statistical experimental design for 250 °C to 400 °C, 2 h up to 5 h time on stream (ToS) and subsequently different residence time besides other parameters. While low temperature (250 °C) promotes cyclohexanol formation from guaiacol, high temperature (400 °C) inhibits hydrogenation, leading to phenol and methane. For medium temperature (340 °C), the selectivity for cyclohexanone increases. Cyclohexanol and cyclohexanone (KA-oil) are the industrial basis for polyamide 6. Furthermore, we clarified the role of 2-methoxycyclohexanol (2MC) in the reaction network towards KA-oil for continuous-mode operation. Statistical analysis was used to predict and optimize product selectivity and yield, leading to the best yield of cyclohexanone/-ol at 327.5 °C, low ToS, medium residence time, high particle dispersity, and medium hydrogen pressure (15 bar(g)).

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控制镍/二氧化硅转化生物油替代愈创木酚的反应网络

用绿色生物油代替化石碳源是向可持续化学工业转变的一条有希望的途径，尽管它们的高氧含量具有挑战性。催化加氢脱氧是将生物油升级为可再生燃料和基础化学品的有利途径。在这项工作中，我们研究了不同金属分散度的Ni/SiO2催化剂在愈创木酚连续模式转化中的作用，采用统计实验设计，在250°C至400°C、2 h至5 h的流上时间(ToS)和随后不同的停留时间(以及其他参数)下进行。低温(250°C)促进愈创木酚生成环己醇，高温(400°C)抑制氢化反应，导致苯酚和甲烷。对于中温(340℃)，环己酮的选择性提高。环己醇和环己酮(ka油)是聚酰胺6的工业基础。此外，我们还明确了2-甲氧基环己醇(2MC)在ka油连续模式反应网络中的作用。结果表明，在327.5℃、低ToS、中等停留时间、高颗粒分散性和中等氢压(15 bar(g))条件下，环己酮/-醇的收率最佳。

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来源期刊

Carbon Resources Conversion Materials Science-Materials Science (miscellaneous)

CiteScore

9.90

自引率

11.70%

发文量

审稿时长

10 weeks

期刊介绍： Carbon Resources Conversion (CRC) publishes fundamental studies and industrial developments regarding relevant technologies aiming for the clean, efficient, value-added, and low-carbon utilization of carbon-containing resources as fuel for energy and as feedstock for materials or chemicals from, for example, fossil fuels, biomass, syngas, CO2, hydrocarbons, and organic wastes via physical, thermal, chemical, biological, and other technical methods. CRC also publishes scientific and engineering studies on resource characterization and pretreatment, carbon material innovation and production, clean technologies related to carbon resource conversion and utilization, and various process-supporting technologies, including on-line or off-line measurement and monitoring, modeling, simulations focused on safe and efficient process operation and control, and process and equipment optimization.