Abstract
Production of biomass-derived sustainable alternative jet fuels (SAJF) has been considered as an important approach to decarbonize the aviation industry but still possesses various challenges in technology advancement, particularly in achieving high carbon efficiency. Here we report a hybrid pathway to SAJF from 2,3-butanediol (2,3-BDO), integrating biologically converting biomass to 2,3-BDO with catalytically upgrading of 2,3-BDO to jet-range hydrocarbons. This pathway is demonstrated to have a high carbon recovery to liquid hydrocarbons from corn stover (25-28%) (74-82% of the theoretical maximum efficiency). The catalytic conversion steps involve 2,3-BDO to C3+ olefins, oligomerization, and hydrogenation where the first two steps are the focus of this study. Under optimum reaction conditions (523 K, 115 kPa, 1.0 h-1 weight hourly space velocity), 2,3-BDO conversion and C3+ olefin selectivity are >97% and 94-98% during 40 h time on stream, respectively. To demonstrate the adaptability of this technology with bio-derived 2,3-BDO, we also investigated the impact of water and other organic coproducts (acetoin and acetic acid) inherited from the fermentation broth on the catalyst performance and product selectivities. We have shown that the catalyst can handle a significant amount of water in the liquid feed (40 wt% water/60 wt% 2,3-BDO) and maintain catalyst stability for ∼40 h. Acetoin can be converted to similar C3+ olefins as 2,3-BDO with complete conversion of acetoin. Co-feeding 10 wt% acetoin with 2,3-BDO is found to have no impact on 2,3-BDO conversion, C3+ olefin selectivity, and catalyst stability. The utilization of organic coproduct like acetoin can help to improve overall carbon conversion efficiency when using real biomass-derived 2,3-BDO. On the other hand, the presence of 10 wt% acetic acid is shown to drastically inhibit methyl ethyl ketone (MEK) hydrogenation and butene oligomerization as revealed by the increased MEK and butene selectivities, implying the importance of separating organic acids when feeding bio-derived 2,3-BDO. The formed C3-C6 olefins from 2,3-BDO are further oligomerized over Amberlyst-36 catalyst to longer-chain hydrocarbons with >70 wt% jet-range hydrocarbons including predominantly iso-olefins/iso-paraffins. The overall carbon efficiency for the jet-range hydrocarbons is 19-22%, exceeding most of the reported biojet pathways, which makes it a promising approach for SAJF production.
| Original language | English |
|---|---|
| Pages (from-to) | 3904-3914 |
| Number of pages | 11 |
| Journal | Sustainable Energy and Fuels |
| Volume | 4 |
| Issue number | 8 |
| DOIs | |
| State | Published - Aug 2020 |
Funding
This research is sponsored by the U.S. Department of Energy (DOE), Office of Energy Efficiency and Renewable Energy, Bio-Energy Technologies Office, under contract DE-AC05-00OR22725 with UT-Battelle, LLC, and in collaboration with the Chemical Catalysis for Bioenergy (ChemCatBio) Consortium, a member of the Energy Materials Network. Microscopy research was supported by the Office of Nuclear Energy, Fuel Cycle R&D Program and the Nuclear Science User Facilities. Funding to NREL was provided by the US Department of Energy, Office of Energy Efficiency and Renewable Energy, Bioenergy Technologies Office under contract No. DE-AC36-08GO28308 with Alliance for Sustainable Energy, LLC, the manager and operator of the National Renewable Energy Laboratory. The author would like to thank Min Zhang and Rick Elander at NREL for discussion on biomass pretreatment, hydrolysis, and fermentation, thank S. K. Reeves at ORNL for assistance with the experimental work and Mi Lu for comments on the manuscript. The views and opinions of the authors expressed herein do not necessarily state or reect those of the United States Government or any agency thereof. A portion of the research mentioned in this study was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. † This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US Government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). ‡ Electronic supplementary information (ESI) available: Scheme, XRD, BET, STEM, TGA, and different reaction results. See DOI: 10.1039/d0se00480d
| Funders | Funder number |
|---|---|
| Bio-Energy Technologies Office | DE-AC05-00OR22725 |
| Chemical Catalysis for Bioenergy | |
| US Department of Energy | |
| U.S. Department of Energy | |
| Office of Energy Efficiency and Renewable Energy |
