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Selective signalling of alcohols by a molecular lattice and mechanism of single-crystal-to-single-crystal transformations
A molecular material undergoes spin-switching as it exchanges MeOH, EtOH or n PrOH with acetone from the lattice. The subsequent thermal single-crystal-to-single-crystal desorption of n PrOH is followed by single crystal X-ray diffraction snapshots.
Sugar-alcohol@ZIF nanocomposites display suppressed phase-change temperatures
The synthesis and characterization of phase change materials infused into metal–organic framework crystals to demonstrate high latent heats with suppressed phase change temperatures.
Economics and global warming potential of a commercial-scale delignifying biorefinery based on co-solvent enhanced lignocellulosic fractionation to produce alcohols, sustainable aviation fuels, and co-products from biomass
First-of-its-kind effort to understand full-scale multi-product biorefineries established upon co-solvent enhanced lignocellulosic fractionation (CELF) from an economic and environmental standpoint.
On the synthesis of biorefineries for high-yield isobutanol production: from biomass-to-alcohol experiments to system level analysis
High yield isobutanol production is experimentally demonstrated. The solvent-to-biomass ratio during pretreatment and enzyme production during hydrolysis are identified as the major economic drivers of the biorefinery.
Substrate Specificity of LACCASE8 Facilitates Polymerization of Caffeyl Alcohol for C-Lignin Biosynthesis in the Seed Coat of Cleome hassleriana
Not Available
Hydroformylation of pyrolysis oils to aldehydes and alcohols from polyolefin waste
Waste plastics are an abundant feedstock for the production of renewable chemicals. Pyrolysis of waste plastics produces pyrolysis oils with high concentrations of olefins (>50 weight %). The traditional petrochemical industry uses several energy-intensive steps to produce olefins from fossil feedstocks such as naphtha, natural gas, and crude oil. In this work, we demonstrate that pyrolysis oil can be used to produce aldehydes through hydroformylation, taking advantage of the olefin functionality. These aldehydes can then be reduced to mono- and dialcohols, oxidized to mono- and dicarboxylic acids, or aminated to mono- and diamines by using homogeneous and heterogeneous catalysis. This route produces high-value oxygenated chemicals from low-value postconsumer recycled polyethylene. Here, we project that the chemicals produced by this route could lower greenhouse gas emissions ~60% compared with their production through petroleum feedstocks.
Correction for Thompson et al., “Fatty Acid and Alcohol Metabolism in Pseudomonas putida : Functional Analysis Using Random Barcode Transposon Sequencing”
Volume 86, no. 21, 2020, e01665-20, https://doi.org/10.1128/AEM.01665-20. Readers should note that when the authors created the deletion mutant of PP_2675, they deleted the entire region between the gene’s start and stop codons. However, this also deleted the DNA that codes for the first 14 amino acids of the overlapping ORF PP_2676. Additionally, the originally published URL for the JBEI public strain repository was incorrect. The correct link to all strains and plasmids in this study is https://public-registry.jbei .org/folders/641.
Engineering Fatty Acid Synthesis in Rhodosporidium Toruloides to Produce Mid-Chain Fatty Acids and Fatty Alcohols (CRADA 501)
C16 Biosciences will partner with NTESS (Sandia National Laboratory) and Pacific Northwest National Laboratory in order to develop microbial technologies for producing sustainable alternatives to palm oil and palm oil derivatives.
Stabilized Open Metal Sites in Bimetallic Metal-Organic Framework Catalysts for Hydrogen Production from Alcohols.
Abstract not provided.
Atomically dispersed supported metal species as catalysts for alcohol conversion, and hydrogen and chemicals production
Supported single metal atoms are a new class of catalyst in which precious metals can be used at the ultimate limit of atom efficiency. While great strides have been made in demonstrating the potential of single-atom catalysts for many industrial reactions, there remains much debate in the literature over the nature of the active sites and the reaction mechanisms. The major goal of this project was to elucidate how atomic dispersions of metals on oxide supports enable catalytic reactions and how to stabilize such active sites for practical catalyst development. This is particularly important for the reactions of interest to fuel reforming for hydrogen generation in which atomically-dispersed metal ions on various oxide surfaces have been identified as the active sites. Working with trace amounts of precious metals is both fundamentally intriguing and of great practical interest in our continual search for low-cost, efficient and stable catalysts for the conversion of fuels to hydrogen under highly demanding operating conditions. A second major goal of the project was to rationally design and prepare single atom alloy (SAA) catalyst compositions based on information gathered from surface science studies on model catalysts and by catalytic evaluation of nanoparticle SAA analogs under realistic conditions. The overarching goal was to use the knowledge garnered from this project to design and develop new catalysts at the single atom limit, which can be applied to selective hydrogenation reactions (alkynes and dienes to alkenes) and the dehydrogenation of methanol and ethanol to value-added products at near-ambient conditions. Detailed information about the results of the project are given below.
Mono-Ether and Alcohol Bioblendstocks to Reduce the Fuel Penalty of Mixing Controlled Compression Ignition (MCCI) Engine Aftertreatment
An integrated approach utilizing catalysis experiments, process systems engineering, fuel property modeling, and engine testing was utilized in this project to optimize the production process and composition of a #2 diesel bioblendstock produced from ethanol consisting primarily of long-chain mono-ethers. The primary objective of the project was to determine the composition and to design the production process for a bioblendstock for #2 diesel fuel with > 50% reduction in greenhouse gas emissions relative to conventional diesel fuel. The desired bioblendstock needed to be blendable with #2 diesel fuel at > 5 vol. % while still meeting ASTM D975 diesel fuel specification properties and achieving improvements in fuel properties: increased cetane number, decreased sooting, and reduced pour point and cloud point temperatures. At the same time, it needed to reduce the fuel energy penalty associated with MCCI engine aftertreatment resulting in improved system efficiency. The findings of the current project demonstrate that primary objective of the work has been met, i.e., to determine the composition and to design the production process for a bioblendstock for #2 diesel fuel with > 50% reduction in greenhouse gas emissions relative to conventional diesel fuel. Additionally, the results indicate that the property objectives (increased cetane number, reduced pour and cloud points, and reduced sooting propensity) for the designed bioblendstock composition have also been met. Engine testing performed has also confirmed that the increased reactivity of the bioblendstock can be used to improve catalyst heating operation and to reduce the fuel penalty associated with this operation mode. The fuel property results demonstrate that >5 vol.% blending is easily achieved while meeting the ASTM D975 #2 diesel fuel property specifications tested in this work, as this was achieved for a blend with 43 vol. % of the bioblendstock. The results provide a foundation for future work to scaleup the catalytic production process designed in this work, with many of the challenges and areas for improvement being identified in this work to enable economic production with low GHG lifecycle emissions.
Fusel Alcohol Fermentation & In Situ Recovery Using Extractive Overlays
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MassIVE MSV000085948 - Utilization of syringyl lignin-derived compounds and production of 2-pyrone-4,6-dicarboxylic acid by Pseudomonas putida KT2440: Lignin is an abundant aromatic polymer formed in plants by coupling reactions of p-coumaryl, coniferyl, and sinapyl alcohols. Pseudomonas putida KT2440 (P. putida KT2440), a robust soil bacterium, naturally catabolizes many aromatic compounds derived from lignin as carbon and energy sources and has been extensively engineered to valorize guaiacyl (G) and p-hydroxyphenyl (H) lignin-derived aromatic species to valuable chemicals. However, only a few studies report the capacity of Pseudomonads to grow on syringyl (S) lignin-derived compounds. In this work, we demonstrate that P. putida KT2440 catabolizes syringate in the presence of an auxiliary energy source. Overexpression of vanAB, encoding a native Rieske non-heme iron monooxygenase, enabled catabolism of syringate and syringaldehyde without an additional carbon and energy source. In vitro biochemical characterization of VanAB confirmed that this enzyme O-demethylates syringate to 3-O-methylgallate and, subsequently, 3-O-methylgallate to gallate, albeit 4- and 55-fold less efficiently than vanillate, respectively. Transcriptomics and proteomics experiments demonstrate that the galADBC transcripts and enzymes required for gallate catabolism are induced when vanAB is overexpressed during cultivation in syringate. Further, we show that that the endogenous protocatechuate-3,4-dioxygenase PcaHG ring-opens gallate to produce 2-pyrone-4,6-dicarboxylic acid (PDC), a promising bio-based chemical. Constitutive overexpression of vanAB and pcaHG along with galA deletion enabled PDC production from SA at a 70% (mol/mol) yield. Furthermore, leveraging the LigAB dioxygenase from Sphingobium sp. SYK-6 and VanAB O-demethylase from Pseudomonas sp. HR199 enabled simultaneous conversion of monomers with S-, G-, and H-type functionality to PDC at 82% (mol/mol) yield. Overall, this study elucidates a native pathway for catabolism of syringyl lignin-derived compounds in P. putida KT2440 and demonstrates the potential of this robust host for biological funneling of substrates derived from all three canonical monolignols.
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The Impact of Carbonation Curing on the Fatigue Behavior of Polyvinyl Alcohol Engineered Cementitious Composites (PVA-ECC)
Use of Engineered Cementitious Composites (ECC) has been proven to enhance structural fatigue resistance and reduce the use-phase emissions for transportation infrastructure. Carbonation curing offers an opportunity to reduce the embodied carbon of ECC via direct CO 2 sequestration. In this study, the impact of carbonation curing on ECC’s fatigue resistance was examined. ECC’s CO 2 uptake, static flexural behavior, flexural fatigue performance, and single fiber pull-out behavior were studied experimentally. Midspan deflection up to 3 million cycles under fatigue load, fatigue stress-life relationship, and failure mechanism for carbonation-cured and air-cured ECC were investigated. Carbonation curing was found to significantly improved the fatigue life of ECC and lowered the midspan deflection under the same stress. Further, CO 2 -cured ECC can achieve >20% CO 2 uptake per cement mass after 24-hour carbonation curing. Carbonation curing increased ECC’s flexural strength by 32% and promoted crack width control capability, with maximum post-fatigue crack width reduced from 148 μm to 76 μm. As a result, the positive impact of carbonation curing on the fatigue behavior of ECC simultaneously lowers the embodied and operational carbon of ECC structural members subjected to fatigue loading during service.
Replication Data for: Exploiting the Liquid Phase to Enhance the Cross-Coupling of Alcohols over Nanoporous Gold Catalysts
The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.
Replication Data for: Predicting a dramatic decline in selectivity for catalytic esterification of alcohols from van der Waals interactions
The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.
The lactate and fusel alcohol platform: Biofuels production and bio/chemical upgrading to advanced biofuels.
Abstract not provided.