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Himmel, Michael E

Publications and source records attributed to Himmel, Michael E.

9 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Ferrous and Ferric Ion-Facilitated Dilute Acid Pretreatment of Lignocellulosic Biomass under Anaerobic or Aerobic Conditions: Observations of Fe Valence Interchange and the Role of Fenton Reaction

Ferrous ion co-catalyst enhancement of dilute-acid (DA) pretreatment of biomass is a promising technology for increasing the release of sugars from recalcitrant lignocellulosic biomass. However, due to the reductive status of ferrous ion and its susceptibility to oxidation with exposure to atmosphere, its effective application presumably requires anaerobic aqueous conditions created by nitrogen gas-purging, which adds extra costs. The objective of this study was to assess the effectiveness of oxidative iron ion, (i.e., ferric ion) as a co-catalyst in DA pretreatment of biomass, using an anaerobic chamber to strictly control exposure to oxygen during setup and post-pretreatment analyses. Remarkably, the ferric ions were found to be as efficient as ferrous ions in enhancing sugar release during DA pretreatment of biomass, which may be attributed to the observation that a major portion of the initial ferric ions were converted to ferrous during pretreatment. Furthermore, the detection of hydrogen peroxide in the liquors after DA/Fe ion pretreatment suggests that Fenton reaction chemistry was likely involved in DA/Fe ion pretreatments of biomass, contributing to the observed ferric and ferrous interchanges during pretreatment. These results help define the extent and specification requirements for applying iron ions as co-catalysts in DA pretreatments of biomass.

09 BIOMASS FUELS↗
DOE OSTI2020

Metabolic engineering of Zymomonas mobilis for anaerobic isobutanol production

Biofuels and value-added biochemicals derived from renewable biomass via biochemical conversion have attracted considerable attention to meet global sustainable energy and environmental goals. Isobutanol is a four-carbon alcohol with many advantages that make it attractive as a fossil-fuel alternative. Zymomonas mobilis is a highly efficient, anaerobic, ethanologenic bacterium making it a promising industrial platform for use in a biorefinery. In this study, the effect of isobutanol on Z. mobilis was investigated, and various isobutanol-producing recombinant strains were constructed. The results showed that the Z. mobilis parental strain was able to grow in the presence of isobutanol below 12 g/L while concentrations greater than 16 g/L inhibited cell growth. Integration of the heterologous gene encoding 2-ketoisovalerate decarboxylase such as kdcA from Lactococcus lactis is required for isobutanol production in Z. mobilis. Moreover, isobutanol production increased from nearly zero to 100-150 mg/L in recombinant strains containing the kdcA gene driven by the tetracycline-inducible promoter Ptet. In addition, we determined that overexpression of a heterologous als gene and two native genes (ilvC and ilvD) involved in valine metabolism in a recombinant Z. mobilis strain expressing kdcA can divert pyruvate from ethanol production to isobutanol biosynthesis. This engineering improved isobutanol production to above 1 g/L. Finally, recombinant strains containing both a synthetic operon, als-ilvC-ilvD, driven by Ptet and the kdcA gene driven by the constitutive strong promoter, Pgap, were determined to greatly enhance isobutanol production with a maximum titer about 4.0 g/L. Finally, isobutanol production was negatively affected by aeration with more isobutanol being produced in more poorly aerated flasks. This study demonstrated that overexpression of kdcA in combination with a synthetic heterologous operon, als-ilvC-ilvD, is crucial for diverting pyruvate from ethanol production for enhanced isobutanol biosynthesis. Moreover, this study also provides a strategy for harnessing the valine metabolic pathway for future production of other pyruvate-derived biochemicals in Z. mobilis.

09 BIOMASS FUELS↗
DOE OSTI2019

Chapter 3.02: Fundamentals and Industrial Applicability of Multifunctional CAZyme Systems

Multifunctional CAZymes have recently garnered a lot of attention due to their high cellulolytic activity, interesting deconstruction mechanisms, intramolecular synergy, and undeniable potential for industrial applications. Here we survey the natural diversity of multifunctional enzymes, especially those identified recently. We discuss the characterization of some of these multifunctional enzymes that can finally be isolated and characterized as full-length constructs, and finally, we review the industrial applicability of these multifunctional enzymes.

09 BIOMASS FUELS↗
DOE OSTI2019

Expression and Characterization of Chimeric CBHI in Yeasts and the Effects of CBHI Fusion to EGII

The low secretion levels of cellobiohydrolaseI (CBHI) in yeasts is one of the key barriers preventing yeast from directly degrading and utilizing lignocellulose. To overcome this barrier, we have explored the approach of genetically linking an easily secreted protein to CBHI, with CBHI being the last to be folded. The Trichoderma reesei eg2 (TrEGII) gene was selected as the leading gene due to its previously demonstrated outstanding secretion in yeast. To comprehensively characterize the effects of this fusion protein, we tested this hypothesis in three industrially relevant yeasts: Saccharomyces cerevisiae, Yarrowia lipolytica, and Lipomyces starkeyi.

09 BIOMASS FUELS↗
DOE OSTI2018

Cellulose–hemicellulose interactions at elevated temperatures increase cellulose recalcitrance to biological conversion

It has been previously shown that cellulose-lignin droplets’ strong interactions, resulting from lignin coalescence and redisposition on cellulose surface during thermochemical pretreatments, increase cellulose recalcitrance to biological conversion, especially at commercially viable low enzyme loadings. However, information on the impact of cellulose–hemicellulose interactions on cellulose recalcitrance following relevant pretreatment conditions are scarce. Here, to investigate the effects of plausible hemicellulose precipitation and re-association with cellulose on cellulose conversion, different pretreatments were applied to pure Avicel® PH101 cellulose alone and Avicel mixed with model hemicellulose compounds followed by enzymatic hydrolysis of resulting solids at both low and high enzyme loadings. Solids produced by pretreatment of Avicel mixed with hemicelluloses (AMH) were found to contain about 2 to 14.6% of exogenous, precipitated hemicelluloses and showed a remarkably much lower digestibility (up to 60%) than their respective controls. However, the exogenous hemicellulosic residues that associated with Avicel following high temperature pretreatments resulted in greater losses in cellulose conversion than those formed at low temperatures, suggesting that temperature plays a strong role in the strength of cellulose–hemicellulose association. Molecular dynamics simulations of hemicellulosic xylan and cellulose were found to further support this temperature effect as the xylan–cellulose interactions were found to substantially increase at elevated temperatures. Furthermore, exogenous, precipitated hemicelluloses in pretreated AMH solids resulted in a larger drop in cellulose conversion than the delignified lignocellulosic biomass containing comparably much higher natural hemicellulose amounts. In conclusion, increased cellulase loadings or supplementation of cellulase with xylanases enhanced cellulose conversion for most pretreated AMH solids; however, this approach was less effective for solids containing mannan polysaccharides, suggesting stronger association of cellulose with (hetero) mannans or lack of enzymes in the mixture required to hydrolyze such polysaccharides.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2017

Biomass Conversion

Biomass constitutes all the plant matter found on our planet, and is produced directly by photosynthesis, the fundamental engine of life on earth. It is the photosynthetic capability of plants to utilize carbon dioxide from the atmosphere that leads to its designation as a 'carbon neutral' fuel, meaning that it does not introduce new carbon into the atmosphere. This article discusses the life cycle assessments of biomass use and the magnitude of energy captured by photosynthesis in the form of biomass on the planet to appraise approaches to tap this energy to meet the ever-growing demand for energy.

09 BIOMASS FUELS↗
DOE OSTI2015

Foreword

The outlook for affordable next-generation or advanced fuels from biomass is as complex and multidimensional as are the possible routes for its attainment.

09 BIOMASS FUELS↗
DOE OSTI2015

Direct Microbial Conversion of Biomass to Advanced Biofuels

'Direct Microbial Conversion of Biomass to Advanced Biofuels' is a stylized text that is rich in both the basic and applied sciences. It provides a higher level summary of the most important aspects of the topic, addressing critical problems solved by deep science. Expert users will find new, critical methods that can be applied to their work, detailed experimental plans, important outcomes given for illustrative problems, and conclusions drawn for specific studies that address broad based issues. A broad range of readers will find this to be a comprehensive, informational text on the subject matter, including experimentalists and even CEOs deciding on new business directions.

09 BIOMASS FUELS↗