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Driving towards cost-competitive biofuels through catalytic fast pyrolysis by rethinking catalyst selection and reactor configuration†
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2018-08-21 00:00:00 , DOI: 10.1039/c8ee01872c
Michael B. Griffin 1, 2, 3 , Kristiina Iisa 1, 2, 3 , Huamin Wang 3, 4, 5 , Abhijit Dutta 1, 2, 3 , Kellene A. Orton 1, 2, 3 , Richard J. French 1, 2, 3 , Daniel M. Santosa 3, 4, 5 , Nolan Wilson 1, 2, 3 , Earl Christensen 1, 2, 3 , Connor Nash 1, 2, 3 , Kurt M. Van Allsburg 1, 2, 3 , Frederick G. Baddour 1, 2, 3 , Daniel A. Ruddy 1, 2, 3 , Eric C. D. Tan 1, 2, 3 , Hao Cai 3, 6, 7 , Calvin Mukarakate 1, 2, 3 , Joshua A. Schaidle 1, 2, 3
Affiliation  

Catalytic fast pyrolysis (CFP) has emerged as an attractive process for the conversion of lignocellulosic biomass into renewable fuels and products. Considerable research and development has focused on using circulating-bed reactors with zeolite catalysts (e.g., HZSM-5) for CFP because of their propensity to form gasoline-range aromatic hydrocarbons. However, the high selectivity for aromatics comes at the expense of low carbon yield, a key economic driver for this process. In this contribution, we evaluate non-zeolite catalysts in a fixed-bed reactor configuration for an integrated CFP process to produce fuel blendstocks from lignocellulosic biomass. These experimental efforts are coupled with technoeconomic analysis (TEA) to benchmark the process and guide research and development activities to minimize costs. The results indicate that CFP bio-oil can be produced from pine with improved yield by using a bifunctional metal-acid 2 wt% Pt/TiO2 catalyst in a fixed-bed reactor operated with co-fed H2 at near atmospheric pressure, as compared to H-ZSM5 in a circulating-bed reactor. The Pt/TiO2 catalyst exhibited good stability over 13 reaction-regeneration cycles with no evidence of irreversible deactivation. The CFP bio-oil was continuously hydrotreated for 140 h time-on-stream using a single-stage system with 84 wt% of the hydrotreated product having a boiling point in the gasoline and distillate range. This integrated biomass-to-blendstock process was determined to exhibit an energy efficiency of 50% and a carbon efficiency of 38%, based on the experimental results and process modelling. TEA of the integrated process revealed a modelled minimum fuel selling price (MFSP) of $4.34 per gasoline gallon equivalent (GGE), which represents a cost reduction of $0.85 GGE−1 compared to values reported for CFP with a zeolite catalyst. TEA also indicated that catalyst cost was a significant factor influencing the MFSP, which informed additional CFP experiments in which lower-cost Mo2C and high-dispersion 0.5 wt% Pt/TiO2 catalysts were synthesized and evaluated. These materials demonstrated CFP carbon yield and oil oxygen content similar to those of the 2 wt% Pt/TiO2 catalyst, offering proof-of-concept that the lower-cost catalysts can be effective for CFP and providing a route to reduce the modelled MFSP to $3.86–3.91 GGE−1. This report links foundational science and applied engineering to demonstrate the potential of fixed-bed CFP and highlights the impact of coupled TEA to guide research activities towards cost reductions.

中文翻译:

通过重新考虑催化剂的选择和反应器配置,通过催化快速热解来推动具有成本竞争力的生物燃料

快速催化热解(CFP)已成为将木质纤维素生物质转化为可再生燃料和产品的有吸引力的方法。大量的研究和开发集中在将循环床反应器与沸石催化剂一起使用(例如,HZSM-5)用于CFP,因为它们易于形成汽油范围的芳烃。然而,对芳烃的高选择性是以低碳收率为代价的,这是该方法的关键经济动力。在此贡献中,我们评估了固定床反应器配置中的非沸石催化剂,以进行整合的CFP工艺以从木质纤维素生物质生产燃料共混原料。这些实验性工作与技术经济分析(TEA)结合在一起,以对过程进行基准测试并指导研发活动以最小化成本。结果表明,通过在共同供料的H 2下运行的固定床反应器中使用2 wt%的双功能金属酸Pt / TiO 2催化剂,可以从松树中生产CFP生物油,并提高产率。与循环床反应器中的H-ZSM5相比,温度接近大气压。Pt / TiO 2催化剂在13个反应-再生循环中表现出良好的稳定性,没有不可逆失活的迹象。使用单级系统对CFP生物油进行连续流加氢处理140小时,其中加氢处理的产品的84 wt%的沸点在汽油和馏出物范围内。根据实验结果和过程建模,该集成的从生物质到混合原料的过程确定显示出50%的能量效率和38%的碳效率。集成过程的TEA显示,模型化的最低燃料销售价格(MFSP)为每汽油加仑当量(GGE)$ 4.34,这意味着成本降低了$ 0.85 GGE -1与报道的使用沸石催化剂的CFP值进行比较。TEA还指出,催化剂成本是影响MFSP的重要因素,这为其他CFP实验提供了参考,在该实验中,合成并评估了低成本Mo 2 C和高分散度0.5 wt%Pt / TiO 2催化剂。这些材料证明了CFP的碳收率和油氧含量与2 wt%Pt / TiO 2催化剂相似,提供了概念证明,即低成本的催化剂可以有效地用于CFP,并提供了减少模型化MFSP的途径至$ 3.86-3.91 GGE -1。该报告将基础科学与应用工程联系起来,以展示固定床CFP的潜力,并着重介绍耦合的TEA对指导研究活动以降低成本的影响。
更新日期:2018-08-21
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