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DOE OSTI2025

Maximizing long-term biohydrogen production with Clostridium thermocellum for high solids conversion of lignocellulosic biomass

Biological hydrogen production from lignocellulosic biomass sustainably couples organic waste reduction with renewable energy generation. Efficient conversion is challenged by the structural complexity of lignocellulose and resulting recalcitrance to enzymatic degradation. Clostridium thermocellum natively breaks down biomass with highly effective hemi-/cellulases systems (i.e., cellulosomes) and generates hydrogen in anaerobic cultivation, creating a compelling platform for lignocellulosic biohydrogen production. Achieving commercially viable production rates requires balancing high biomass loading and throughput against uniform mixing conditions required for enzyme dispersion, pH and temperature control, and efficient hydrogen and metabolite removal in continuous operation. To address these barriers to process intensification, we implemented novel reactor and process designs for high-solids lignocellulosic biomass fermentations using the C. thermocellum KJC19-9 strain, genetically engineered for co-utilization of cellulose and hemicellulose sugars (i.e., xylose). Via computational fluid dynamics (CFD) modeling and experimental validation, we achieved a >50% improvement in biohydrogen production with an improved anchor-type impeller morphology, coupled to a threefold reduction in agitation rate. To further reduce rheological constraints and accumulation of toxic metabolites, we then transitioned the process to sequencing fed-batch operation. The resulting process generated 24.87 L H 2 L −1 from 160 g L −1 of deacetylated and mechanically refined (DMR)-pretreated corn stover biomass over 16 days while solubilizing >95% of influent cellulose and hemicellulose, setting a new performance benchmark for continuous production of biohydrogen from lignocellulose.

08 HYDROGEN↗

DOE OSTI2023

Reversible Iron Oxyfluoride (FeOF)–Graphene Composites as Sustainable Cathodes for High Energy Density Lithium Batteries

Two large barriers are impeding the wide implementation of electric vehicles, namely driving-range and cost, primarily due to the low specific energy and high cost of mono-valence cathodes used in lithium-ion batteries. Iron is the ideal element for cathode materials considering its abundance, low cost and toxicity. However, the poor reversibility of (de)lithiation and low electronic conductivity prevent iron-based high specific energy multi-valence conversion cathodes from practical applications. In this work, a sustainable FeOF nanocomposite is developed with extraordinary performance. The specific capacity and energy reach 621 mAh g –1 and 1124 Wh kg –1 with more than 100 cycles, which triples the specific capacity, and doubles the specific energy of current mono-valence intercalation LiCoO 2 . This is the result of an effective approach, combing the nanostructured FeOF with graphene, realized by making the (de)lithiation reversible by immobilizing FeOF nanoparticles and the discharge products over the graphene surface and providing the interparticle electric conduction. Importantly, it demonstrates that introducing small amount of graphene can create new materials with desired properties, opening a new avenue for altering the (de)lithiation process. Finally, such extraordinary performance represents a significant breakthrough in developing sustainable conversion materials, eventually overcoming the driving range and cost barriers.

25 ENERGY STORAGE↗

DOE OSTI2021

Insights into the Enhanced Oxidative Thermal Stability of Nanoparticle Organic Hybrid Materials Developed for Carbon Capture and Energy Storage

Due to the growing need for Direct Air Capture (DAC) and integrated carbon capture and conversion technologies, CO 2 capture materials that can withstand a wide range of environmental conditions, including fluctuating ambient temperatures and high concentrations of oxidizing agents (i.e., oxygen and moisture), are critically needed. Liquid-like Nanoparticle Organic Hybrid Materials (NOHMs) have been proposed as candidates for DAC and electrolyte additives enabling sustainable energy storage (i.e., integrated CO 2 capture and conversion and flow batteries). Liquid-like NOHMs functionalized with an ionic bond have been shown to display greatly enhanced oxidative thermal stability compared to the untethered polymer. However, these studies were limited in terms of reaction conditions and the detailed mechanisms of the oxidative thermal degradation were not reported. In this work, a kinetic thermal degradation analysis was performed on NOHM-I-HPE and the neat polymer, Jeffamine M2070 (HPE), in both non-oxidative and oxidative conditions. NOHM-I-HPE displayed similar thermal stability to the untethered polymer in a nitrogen environment, but interestingly, the thermal stability of the ionically tethered polymer was significantly enhanced in the presence of air. This observed enhancement of oxidative thermal stability is attributed to the orders of magnitude larger viscosity of the liquid-like NOHMs compared to untethered polymer and the bond stabilization of the ionically tethered polymer in the NOHMs canopy. Further, spectroscopic analyses of the liquid residue revealed that in the presence of oxygen, the degradation of HPE and NOHM-I-HPE occurs through the formation of trace amounts of carbonyls. This study illustrated that NOHMs can serve as functional materials for sustainable energy storage applications because of their excellent oxidative thermal stability.

25 ENERGY STORAGE↗

DOE OSTI2020

Insights into Mechanisms of Screw Feeder Plugging by Heated Pine Forestry Residues Using in-situ and Correlative Microscopy

Increasing concerns about global carbon emissions due to fossil fuel use has created interest in renewable fuel alternatives, such as lignocellulosic biomass. With an estimated global biomass production probability ten-fold higher than projected need, functionalizing and scaling biomass conversion processes, like pyrolysis, is a promising component of a diverse sustainable energy program (Kan, Strezov, & Evans, 2016). Pyrolysis reactors employed in biomass conversion often encounter the known problem of screw feeder plugging, halting work and reducing efficiency of biorefineries. Although the screw feeder is not heated directly, conductive heat transfer from the fluidized bed pyrolysis reactor creates a temperature gradient, where particles experience temperatures between 22°C and 500°C from the time they enter the feeder to being emptied into the reactor (Digman, Joo, & Kim, 2009; Nieminen & Folke, 1982). The impact of unintentional heating on this highly variable feedstock may result in particle morphology modification, surface texture transformation, and the evolution of viscous compounds and may contribute to screw feeder plugging (Haas, Nimlos, & Donohoe, 2009; Ingram et al., 2008). We hypothesized that particles of various anatomical fractions (including needles, branches, bark, cambium, and whitewood) will experience dramatic changes during this heating regime, which will be characterized by decreased particle size, increased surface roughness, degradation of key structural macromolecules, and generation of viscous compounds that would result in increased particle friction and cohesion, contributing to screw feeder plugging.

biofuels↗

DOE OSTI2025

Process and environmental safety of thermochemical conversion of biomass

Biomass presents a promising opportunity for converting waste into valuable energy, fuels, and chemicals through various thermochemical processes, including hydrothermal carbonization, hydrothermal liquefaction, pyrolysis, gasification, and combustion. However, these processes operate under extreme conditions, introducing significant safety hazards that necessitate meticulous management to prevent accidents. This review discusses potential hazards, risk mitigation strategies, and safety management practices, emphasizing the importance of integrated safety measures into the design and operation of these processes. It also highlights the critical need for robust safety engineering and environmental management strategies tailored to each thermo-chemical process. As these processes transition from laboratory to industrial scale, there is an imperative to develop a clear and concise pathway for emerging industries to achieve regulatory compliance, achieve safety certification, and enable effective stewardship of potential fugitive emissions. By addressing safety and environmental concerns, stakeholders can optimize economic benefits, rural development, and achieve sustained domestic energy generation benefits offered by biomass conversion technologies. Further research on plant design optimization, operational safety, environmental evaluation standardization, and innovative waste management solutions will support the safe and effective scaling of these technologies, ultimately contributing to sustainable management and resource recovery.

09 - BIOMASS FUELS↗

DOE OSTI2021

Root water uptake of biofuel crops revealed by coupled electrical resistivity and soil water content measurements

Abstract Biofuel crops, including annuals such as maize ( Zea mays L.), soybean [ Glycine max (L.) Merr.], and canola ( Brassica napus L.), as well as high‐biomass perennial grasses such as miscanthus ( Miscanthus × giganteus J.M. Greef & Deuter ex Hodkinson & Renvoiz), are candidates for sustainable alternative energy sources. However, large‐scale conversion of croplands to perennial biofuel crops could have substantial impacts on regional water, nutrient, and C cycles due to the longer growing seasons and differences in rooting systems compared with most annual crops. However, due to the limited tools available to nondestructively study the spatiotemporal patterns of root water uptake in situ at field scales, these differences in crop water use are not well known. Geophysical imaging tools such as electrical resistivity (ER) reveal changes in water content in the soil profile. In this study, we demonstrate the use of a novel coupled hydrogeophysical approach with both time domain reflectometry soil water content and ER measurements to compare root water uptake and soil properties of an annual crop rotation with the perennial grass miscanthus, across three growing seasons (2009–2011) in southwest Michigan, USA. We estimated maximum root depths to be between 1.2 and 2.2 m, with the vertical distribution of roots being notably deeper in 2009 relative to 2010 and 2011, likely due to the drought conditions during that first year. Modeled cumulative ET of both crops was underestimated (2–34%) relative to estimates obtained from soil water drawdown in prior studies but was found to be greater in the perennial grass than the annual crops, despite shallower modeled rooting depths in 2010 and 2011.

Kuhl, Alexandria S.↗

DOE OSTI2021

Circular Bioeconomy Concepts—A Perspective

Circular economy concepts—including a circular bioeconomy—aim to transition the current, essentially linear, economic system to a more sustainable one. However, organizations and researchers currently define the circular economy concept differently, resulting in inconsistencies and difficulty in effectively implementing the framework. In this paper, we provide our perspective on the conceptual definitions of the circular economy, bioeconomy, and circular bioeconomy, outlining potential overlaps and differences and proposing a harmonized interpretation that stresses the importance of the carbon cycle. We conclude that the key goal of a circular economy is to slow, narrow, and close material resource loops, built on the foundation of renewable energy and non-toxic materials. Further, a sustainable bioeconomy goes beyond simply switching fossil resources with renewable, biological resources. It requires low-carbon energy inputs, sustainable supply chains, and promising disruptive conversion technologies for the sustainable transformation of renewable bioresources to high-value bio-based products, materials, and fuels. The bio-based circular carbon economy, in particular, stresses capturing atmospheric carbon via photosynthesis and exploiting this unique feature to the fullest extent possible. It sits at the intersection between the circular economy and the bioeconomy concept, resulting in a framework that focuses on closing the carbon cycle and stressing the opportunity to create an additional carbon sink capability in the technosphere by utilizing biogenic carbon for products and materials that are circulated in same or improved use cycles. Lastly, a sustainable circular bioeconomy transition will necessitate a set of consistent metrics that fit all products and industries.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2022

Metal-Supported Solid Oxide Fuel Cells for Natural Gas

Solid oxide fuel cells (SOFCs) are high temperature energy conversion devices that produce electricity efficiently and sustainably. High operating temperatures required for SOFC function endow these devices with many advantages including fuel flexibility and high conversion efficiencies. Fuel flexibility, in particular, distinguishes SOFCs from other types of fuel cells that operate with clean H 2 only, and enables operation with natural gas (NG). LBNL has developed metal supported SOFCs (MS-SOFCs) with unique symmetrical architecture that offer several advantages over state of the art (SoA) ceramic SOFC models including inexpensive materials, rapid start up capability, increased mechanical strength and high tolerance to thermal cycling, Fig 1. These advantages make LBNL MS-SOFCs uniquely suited for fast start-up, portable, and mobile backup generator applications. Specifically motivating this work was a scenario of backup generators fueled by pipeline natural gas delivered from SoCalGas in the event of an electric grid shut down. This project investigates the feasibility of using MS-SOFCs with pre-reformed natural gas as well as direct on-cell reforming of simulated natural gas both with and without sulfur.

03 NATURAL GAS↗

DOE OSTI2022

Forum on Materials and Interfaces for Energy Storage and Conversion

This ACS Applied Materials & Interfaces forum on energy storage and conversion contains the topics of research discoveries to advance energy technology development. The topics are focused on the efficient and sustainable use of energy in the fields of fuel cells, CO 2 conversion, water splitting, batteries, and electrochemical capacitor. This forum highlights recent achievements in these emerging technologies through the design and evaluation of novel materials and devices and theoretical study. Additionally, this forum also showcases the technology at all stages of development from “embryonic” conception to industrial adaptation.

25 ENERGY STORAGE↗

DOE OSTI2021

Metal Oxide-Induced Instability and Its Mitigation in Halide Perovskite Solar Cells

Halide perovskite solar cells (PSCs) have emerged as a promising photovoltaic technology for sustainable energy solutions due to their impressive power conversion efficiency and a path to be manufactured by low-cost, high-throughput methods. To reach PSCs’ full potential for practical implementation, it is crucial to solving the issues related to its long-term operational stability. Furthermore, given that PSCs consist of many layers of dissimilar materials which form multiple internal interfaces, it is prudent to examine whether there exist interfacial interactions, most importantly between transport layers and perovskite absorbers, that can trigger device performance and instability. In this perspective, we bring to the attention of the PSC research community the lesser-known interfacial degradation of halide perovskites promoted by contact with metal oxide transport layers and highlight the deleterious effects on the PSCs’ performance and stability. We also discuss various mitigation strategies that have shown promises to achieve high-performing and stable PSCs.

14 SOLAR ENERGY↗

DOE OSTI2023

Co 2 Mo 6 S 8 Catalyzes Nearly Exclusive Electrochemical Nitrate Conversion to Ammonia with Enzyme-like Activity

Electrocatalytic nitrate to ammonia conversion is a key reaction for energy and environmental sustainability. This reaction involves complex multi electron and proton transfer steps, and is impeded by the lack of catalyst for promoting both reactivity and ammonia selectivity. Here, we demonstrate active motifs based on the Chevrel phase Co 2 Mo 6 S 8 exhibit an enzyme-like high turnover frequency of ~95.1 s –1 for nitrate electroreduction to ammonia. We reveal strong synergy of multiple binding sites on this catalyst, such that the ligand effect of Co steers H ad* toward hydrogenation other than hydrogen evolution, the ensemble effect of Co, and the spatial confinement effect that promote the full hydrogenation of NO x to ammonia without N–N coupling. The catalyst exhibits almost exclusive ammonia conversion with a Faradaic efficiency of 97.1% and ammonia yielding rate of 115.5 mmol·g cat –1 ·h –1 in neutral electrolytes. The high activity was also confirmed in electrolytes with dilute nitrate and high chloride concentrations.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Solar energy conversion by photosystem II: principles and structures

Photosynthetic water oxidation by Photosystem II (PSII) is a fascinating process because it sustains life on Earth and serves as a blue print for scalable synthetic catalysts required for renewable energy applications. The biophysical, computational, and structural description of this process, which started more than 50 years ago, has made tremendous progress over the past two decades, with its high-resolution crystal structures being available not only of the dark-stable state of PSII, but of all the semi-stable reaction intermediates and even some transient states. Here, we summarize the current knowledge on PSII with emphasis on the basic principles that govern the conversion of light energy to chemical energy in PSII, as well as on the illustration of the molecular structures that enable these reactions. The important remaining questions regarding the mechanism of biological water oxidation are highlighted, and one possible pathway for this fundamental reaction is described at a molecular level.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Modeling Planar Electrodes and Zero–Gap Membrane Electrode Assemblies for CO 2 Electrolysis

Multiphysics modeling enables probing of conditions inside a CO 2 electrolyzer that are difficult to measure, such as local concentrations and pH, as well as rapid testing of possible design changes. A one-dimensional model for a zero-gap membrane electrode assembly (MEA) CO 2 electrolyzer was developed with the assumption that catalyst layers interact with the membrane ionomer such that the ionomer affects the underlying kinetics. The kinetics for bicarbonate reacting to form hydrogen are fit using a planar electrode model for silver with an ionomer coating. The MEA model results are validated against experimental studies for current density and product selectivity. Flooding of the cathode is modeled using saturation curves, and results show that blocked pores in the microporous layer play a significant role in limiting the mass transport at high potentials (>2.8 V). Sensitivity studies showed that CO Faradaic efficiency can be increased by decreasing catalyst layer thickness and porosity, and decreasing KHCO 3 concentration.

30 DIRECT ENERGY CONVERSION↗

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 OSTI2024

SAE Government-Industry - Heavy-Duty Policy: Panel Discussion (G203)

Medium- and heavy-duty vehicles are 21% of US transportation greenhouse gas (GHG) emissions and a major source of air pollution. In this talk to present some results exploring how the total cost of driving (TCD) of zero-emission vehicles (ZEVs), including battery electric vehicles and hydrogen fuel cell electric vehicles (EVs and FCEVs), could evolve under alternative scenarios. Results show that with continued improvements in vehicles and fuels, ZEVs can rapidly become viable, potentially reaching TCD parity or better compared to diesel vehicles by 2035 for all market segments. For heavy long-haul trucks, EVs become competitive on a TCD basis at charging costs below $0.18/kWh, while FCEVs become competitive on a TCD basis at hydrogen costs below $5/kg. A full transition to ZEV sales by 2035 results in 65% emissions reductions by 2050 compared to 2019 without supportive policies. Incentives such as the Inflation Reduction Act vehicle purchase credits further accelerate ZEV TCD competitiveness with major adoption opportunities over the next five years.

ADVANCED PROPULSION SYSTEMS,DIRECT ENERGY CONVERSI↗

DOE OSTI2023

2023 Roadmap on molecular modelling of electrochemical energy materials

New materials for electrochemical energy storage and conversion are the key to the electrification and sustainable development of our modern societies. Molecular modelling based on the principles of quantum mechanics and statistical mechanics as well as empowered by machine learning techniques can help us to understand, control and design electrochemical energy materials at atomistic precision. Therefore, this roadmap, which is a collection of authoritative opinions, serves as a gateway for both the experts and the beginners to have a quick overview of the current status and corresponding challenges in molecular modelling of electrochemical energy materials for batteries, supercapacitors, CO 2 reduction reaction, and fuel cell applications.

25 ENERGY STORAGE↗

DOE OSTI2024

Sustainable Valorization of CO2 through Nuclear Power-to-X Pathways

Some of the issues concerning energy security and climate change can be addressed by employing nuclear power (NP) to supply the energy required for the conversion of carbon dioxide (CO2) into chemicals, products, and materials. Nuclear energy represents a neutral carbon source that can be generated sustainably, reliably, and consistently. Nuclear power plants (NPPs) could supply energy in the form of heat, electricity, and ionizing radiation to drive CO2 chemical reactions underpinning NP-to-X type of pathways. CO2 conversion processes are either commercially available or emerging technologies at different developmental maturity stages. This work reviews the published literature (articles and patents) that reports R&D results and the understanding and development of chemical reactions and processes, as well as the efforts in integrating NPPs and chemical processes (CPs). As will be made evident, a new industrial era for the manufacturing of decarbonized chemicals, products, and materials will be possible by developing and implementing new (more energy- and carbon-efficient) processes responding to the NP-to-X pathways. This new decarbonizing platform not only contributes to achieving net zero goals but also broadens the NPP product beyond electricity.

08 HYDROGEN↗

DOE OSTI2023

Supply Chain Sustainability Analysis of Renewable Hydrocarbon Fuels via Hydrothermal Liquefaction, Combined Algal Processing, and Biochemical Conversion: Update of the 2022 State-of-Technology Cases

The Department of Energy's (DOE) Bioenergy Technologies Office (BETO) aims to develop and deploy technologies to transform renewable biomass resources into commercially viable, high-performance biofuels, bioproducts, and biopower through public and private partnerships. BETO and its national laboratory teams conduct in-depth techno-economic assessments (TEA) of biomass feedstock supply and logistics and conversion technologies to produce biofuels. There are two general types of TEAs: A design case outlines a target case (future projection) for a particular biofuel pathway. It informs R&D priorities by identifying areas in need of improvement, tracks sustainability impact of R&D, and provides goals and benchmarks against which technology progress is assessed. A state of technology (SOT) analysis assesses progress within and across relevant technology areas based on actual results at current experimental scales relative to technical targets and cost goals from design cases, and includes technical, economic, and environmental criteria as available. In addition to developing a TEA for a pathway of interest, BETO also performs a supply chain sustainability analysis (SCSA). The SCSA takes the life-cycle analysis approach that BETO has been supporting for over 20 years. It enables BETO to identify energy consumption, environmental, and sustainability issues that may be associated with biofuel production. Approaches to mitigating these issues can then be developed. Additionally, the SCSA allows for comparison of energy and environmental impacts across biofuel pathways in BETO's research and development portfolio. This technical report describes the SCSAs for the production of renewable hydrocarbon transportation fuels via a range of conversion technologies in the 2022 SOTs: (1) renewable hydrocarbon fuels via hydrothermal liquefaction (HTL) of wet sludge from a wastewater treatment plant; (2) renewable hydrocarbon fuels via biochemical conversion of herbaceous lignocellulosic biomass; (3) renewable hydrocarbon fuels via HTL of an algae/woody biomass blend; and (4) renewable hydrocarbon fuels via combined algae processing (CAP).

09 BIOMASS FUELS↗