Advancements and challenges in the production of low-carbon fuels via catalytic fast pyrolysis of biomass through refinery integration and co-product generation†

IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Green Chemistry Pub Date : 2023-08-07 DOI:10.1039/D3GC01574B
Matthew M. Yung, Calvin Mukarakate, Kristiina Iisa, A. Nolan Wilson, Mark R. Nimlos, Susan E. Habas, Abhijit Dutta, Kinga A. Unocic, Joshua A. Schaidle and Michael B. Griffin
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Abstract

The production of advanced biofuels represents a near-term opportunity to decarbonize the heavy vehicle transportation sector. However, important barriers must be overcome and successful deployment of these technologies will require (i) catalyst and process development to reduce cost and improve carbon utilization and (ii) industry-relevant validation of operability to de-risk scale-up. Herein, we seek to address these challenges for an integrated two-step process involving catalytic fast pyrolysis (CFP) followed by co-hydrotreating of bio-oil with refinery streams. Technoeconomic and lifecycle analysis based on the data presented herein reveal the potential to generate low-carbon transportation fuels and chemical co-products with a modelled selling price of $2.83 gasoline gallon equivalent (2016$) and a 78% reduction in greenhouse gas emissions compared to fossil-based pathways. The feedstock for this research was a blend of 50 wt% loblolly pine and 50 wt% waste forest residues, and the CFP step was performed using an ex situ fixed bed of Pt/TiO2 with co-fed H2 at atmospheric pressure. Compared to previous state-of-technology benchmarks, advancements in catalyst design and synthesis methodology enabled a four-fold reduction in Pt loading and a 400% increase in time on stream without negatively impacting upgrading performance. Additionally, a first-of-its-kind integrated assessment of waste gas adsorption showed near quantitative recovery of acetone and 2-butanone, which collectively represent approximately 5% of the biomass carbon. The valorization of these co-products opens opportunities to support decarbonization of the chemical sector while simultaneously improving the overall process carbon efficiency to >40%. After condensation, the CFP-oil was co-hydrotreated with straight run diesel (10 : 90 vol%) to achieve 95% biogenic carbon incorporation. The oxygen content of the hydrotreated oil was below detection limits, and the diesel fraction exhibited a cetane number and cloud point suitable for a finished fuel. This manuscript concludes by highlighting remaining research needs associated with improving thermal management during catalyst regeneration, mitigating catalyst deactivation due to inorganic deposition, and demonstrating the durability of biomass feeding systems when operated in hydrogen-rich environments.

Abstract Image

通过炼油厂整合和副产品生成生物质催化快速热解生产低碳燃料的进展和挑战
先进生物燃料的生产代表了重型车辆运输部门脱碳的近期机会。然而,必须克服重要的障碍,这些技术的成功部署将需要(i)催化剂和工艺开发,以降低成本和提高碳利用率;(ii)与行业相关的可操作性验证,以减少风险的扩大。在此,我们寻求解决这些挑战的集成两步工艺,包括催化快速热解(CFP),然后与炼油厂流共加氢处理生物油。基于本文提供的数据的技术经济和生命周期分析表明,与化石燃料相比,低碳运输燃料和化学副产品的模型售价为2.83美元汽油加仑当量(2016年美元),温室气体排放量减少78%。本研究的原料是50%火炬松和50%森林废弃物的混合物,CFP步骤是在常压下使用Pt/TiO2的非原位固定床和共进料H2进行的。与之前的技术基准相比,催化剂设计和合成方法的进步使Pt负载减少了4倍,生产时间增加了400%,而不会对升级性能产生负面影响。此外,对废气吸附的首次综合评估显示,丙酮和2-丁酮的回收率接近定量,它们总共约占生物质碳的5%。这些副产品的增值为支持化工行业的脱碳提供了机会,同时将整个过程的碳效率提高到40%。冷凝后,cfp油与直馏柴油(10:90 vol%)共加氢处理,达到95%的生物炭掺入率。加氢处理后的油氧含量低于检测限值,柴油馏分呈现出适合成品燃料的十六烷值和浊点。本文最后强调了与改善催化剂再生过程中的热管理、减轻无机沉积引起的催化剂失活以及在富氢环境中运行时生物质投料系统的耐久性相关的剩余研究需求。
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来源期刊
Green Chemistry
Green Chemistry 化学-化学综合
CiteScore
16.10
自引率
7.10%
发文量
677
审稿时长
1.4 months
期刊介绍: Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.
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