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DOE OSTI2024

Nanochannel electrodes facilitating interfacial transport for PEM water electrolysis

Proton-exchange membrane water electrolyzers (PEMWEs) are a promising technology for green hydrogen production; however, interfacial transport behaviors are poorly understood, hindering device performance and longevity. Here, we first utilized finite-gap electrolyzer to demonstrate the possibility of proton transfer through water in PEMWEs. The measured high-frequency resistances (HFRs) exhibit a linear trend with increasing gap distance, where extrapolation shows a lower value compared with HFRs in regular zero-gap electrolyzers, indicating that ohmic resistance could be further reduced. We introduce nanochannels to facilitate mass transport, as evidenced by both liquid-fed and vapor-fed electrolysis. Nanochannel electrodes achieve a voltage reduction of 190 mV at 9 A·cm –2 compared with the Ir-PTEs without nanochannels. Furthermore, nanochannel electrodes show negligible degradation through 100,000 accelerated-stress tests and over 2,000 h of operation at 1.8 A·cm –2 with a decay rate of 11.66 μV·h –1 . These results provide new insights into localized transport dynamics for PEMWEs and highlight the significance of interfacial engineering for electrochemical devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Spectroscopic Characterization of Mn 1+ Low Oxidation State in Prussian Blue-Based Battery Anodes

Stabilization of ions in exotic oxidation states is beneficial for the development of new materials for green energy technologies. Exotic Mn 1+ was proposed to play a role in the function of sodium-based Prussian blue analogues (PBA) batteries, a highly sought-out technology for industrial energy storage. Here, we report the detailed electronic structure characterization of uncharged and charged sodium-based manganese hexacyanomanganate anodes via Mn K-edge X-ray absorption spectroscopy (XAS), Kβ nonresonant X-ray emission (XES), and resonant inelastic X-ray scattering (RIXS). The latter allowed us to obtain site-selective XANES information about two distinct Mn centers. The obtained spectroscopic data represent the first electronic structure characterization of low-spin Mn 1+ using hard X-ray RIXS and XES and allowed us to confirm its role in anode reduction. In conclusion, our experimental approach can be expanded to analysis of analogues with other 3d transition metals broadening the application of exotic ionic states in materials engineering.

36 MATERIALS SCIENCE↗

DOE OSTI2023

A High-Entropy Oxide as High-Activity Electrocatalyst for Water Oxidation

High-entropy materials are an emerging pathway in the development of high-activity (electro)catalysts because of the inherent tunability and coexistence of multiple potential active sites, which may lead to earth-abundant catalyst materials for energy-efficient electrochemical energy storage. In this report, we identify how the multication composition in high-entropy perovskite oxides (HEO) contributes to high catalytic activity for the oxygen evolution reaction (OER), i.e., the key kinetically limiting half-reaction in several electrochemical energy conversion technologies, including green hydrogen generation. We compare the activity of the (001) facet of LaCr 0.2 Mn 0.2 Fe 0.2 Co 0.2 Ni 0.2 O 3-δ with the parent compounds (single B-site in the ABO 3 perovskite). While the single B-site perovskites roughly follow the expected volcano-type activity trends, the HEO clearly outperforms all of its parent compounds with 17 to 680 times higher currents at a fixed overpotential. As all samples were grown as an epitaxial layer, our results indicate an intrinsic composition–function relationship, avoiding the effects of complex geometries or unknown surface composition. In-depth X-ray photoemission studies reveal a synergistic effect of simultaneous oxidation and reduction of different transition metal cations during the adsorption of reaction intermediates. The surprisingly high OER activity demonstrates that HEOs are a highly attractive, earth-abundant material class for high-activity OER electrocatalysts, possibly allowing the activity to be fine-tuned beyond the scaling limits of mono- or bimetallic oxides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Accelerating the discovery of novel magnetic materials using machine learning–guided adaptive feedback

Magnetic materials are essential for energy generation and information devices, and they play an important role in advanced technologies and green energy economies. Currently, the most widely used magnets contain rare earth (RE) elements. An outstanding challenge of notable scientific interest is the discovery and synthesis of novel magnetic materials without RE elements that meet the performance and cost goals for advanced electromagnetic devices. Here, we report our discovery and synthesis of an RE-free magnetic compound, Fe 3 CoB 2 , through an efficient feedback framework by integrating machine learning (ML), an adaptive genetic algorithm, first-principles calculations, and experimental synthesis. Magnetic measurements show that Fe 3 CoB 2 exhibits a high magnetic anisotropy ( K 1 = 1.2 MJ/m 3 ) and saturation magnetic polarization ( J s = 1.39 T), which is suitable for RE-free permanent-magnet applications. Our ML-guided approach presents a promising paradigm for efficient materials design and discovery and can also be applied to the search for other functional materials.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Influence of Supporting Electrolyte on Hydroxide Exchange Membrane Water Electrolysis Performance: Catholyte

Alkaline or hydroxide exchange membrane water electrolysis (HEMWE) is a promising technology for green hydrogen production using platinum group metal-free catalysts and stainless steel, an advantage of alkaline water electrolysis (AWE), and a gas-impermeable membrane, a parallel to proton exchange membrane electrolysis (PEMWE). However, the HEMWE requires supporting electrolytes and there is minimal understanding of their role on the respective reactions. Without SELs, HEMWE performance and durability are worse than PEMWE systems. Herein, consistently feeding potassium hydroxide anolyte, we systematically study the effects of catholyte SELs in HEMWEs including dry vs. wet operation, cation effects, anion effects, and cation/OH ratios on cell potential and stability. We report that (i) hydration of the cathode improves high current density operation by preventing dehydration of the hydroxide exchange membrane (HEM), (ii) there was no correlation between cation type and cell potential, (iii) cell potential and high frequency resistance did not correlate with SEL conductivity, (iv) cathodic carbonate SEL had a significant negative effect on cell performance, (v) increased cation/OH ratio also caused increased cell potentials. Overall, this study concludes that feeding water or potassium hydroxide solution is desirable to improve the AEMWE performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Reports From The Frontier: Overcoming Limitations for Pure-water Anion-exchange-membrane Electrolysis

Anion-exchange-membrane electrolysis is positioned to play a key role in the predicted exponential growth of green hydrogen technology with essential R&D advances. We reveal key design parameters essential to commercialization. First, stable alkaline oxygen-evolution reaction catalysts with high electronic conductivity and minimal surface reconstruction during operation must be designed. Alkaline catalyst layers must also be applied to the membrane electrode assembly with scalable, industrially relevant techniques. Second, ionomer oxidation mitigation strategies must be developed. Furthermore, this approach could also target other creative catalyst layer design, such as phase-separation control to protect oxidation-prone organic components or catalyst engineering to direct selectivity for hydroxide over polymer oxidation. If competitive efficiency and durability can be achieved in pure water, AEM electrolysis has the potential to become a dominant electrolyzer technology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Self-Disinfecting PPE Fabric [Factsheet]

Green Theme Technologies Inc. developed a chemical finishing technology that uses a high pressure, water-free, thermally triggered polymerization process to produce a thin conformal polymer coating around fabric fibers. This process can be used to embed selective, disinfectant chemicals to provide an anti-microbial, anti-viral finish to fabrics. In the face of COVID-19, the company hopes this process produces a permanent, laundry-durable, anti-pathogenic finish. Essentially, creating regenerative and reusable PPE.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Development and Commercialization of a Nanosegrated Oxygen Evolution Reaction Electrocatalyst (CRADA)

This collaborative project leverages advanced characterization tools, catalyst treatment and electrochemical testing capabilities at LBNL to help commercialize a bimetallic nanosegrated catalysts for oxygen evolution reaction in proton-exchange membrane water electrolyzers. This project also has three industrial partners who are involved in catalyst scale-up synthesis, large electrode fabrication and large electrode electrochemical testing. This project investigates a broad range of topics including electrocatalysis, ink rheology and electrode fabrication and testing. This knowledge could help bridge the performance and durability gap from laboratory-developed materials (such as electrocatalysts) to applications in commercial devices. The research results also bring fundamental understanding of possible degradation mechanisms that occur under extremely oxidative potentials including material and morphological changes. The project will help accelerate the deployment of proton-exchange membrane water electrolyzers. The public benefits could include creating jobs and increasing public awareness of potential clean technologies for green hydrogen production. Ultimately, the project will help national wide effort of flighting climate change and achieving carbon neutrality by 2050.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2021

Lithium Metal as an Anode in Electrochemical Energy Storage

The drastic environmental and economic costs of global warming have driven the necessity to reduce, if not eliminate, a dependency on oil and gas for energy applications. Alternative clean energy reliance has been initiated as a global investment for a more sustainable future. Part of this transitional effort is focused on energy storage via a rechargeable battery. High energy density storage is necessary for utilizing non-dispatchable green energy technologies, as well in the electric transition of our vehicle fleet. Further, understanding methods of extracting, manufacturing, and recycling lithium is necessary to lessen environmental impact. Lithium metal is often considered the “Holy Grail” of battery technology, due to its high theoretical capacity (3,860 mAh/g) and low electrochemical potential (-3.04 V vs. SHE). However, parasitic reactions lead to rapid and dangerous battery failure. Therefore, determining methods of stabilizing lithium metal is paramount for the transition to a greener future.

25 ENERGY STORAGE↗

DOE OSTI2024

Photocatalytic water splitting for large-scale solar-to-chemical energy conversion and storage

Sunlight-driven water splitting allows renewable hydrogen to be produced from abundant and environmentally benign water. Large-scale societal implementation of this green fuel production technology within energy generation systems is essential for the establishment of sustainable future societies. Among various technologies, photocatalytic water splitting using particulate semiconductors has attracted increasing attention as a method to produce large amounts of green fuels at low cost. The key to making this technology practical is the development of photocatalysts capable of splitting water with high solar-to-fuel energy conversion efficiency. Furthermore, advances that enable the deployment of water-splitting photocatalysts over large areas are necessary, as is the ability to recover hydrogen safely and efficiently from the produced oxyhydrogen gas. This lead article describes the key discoveries and recent research trends in photosynthesis using particulate semiconductors and photocatalyst sheets for overall water splitting, via one-step excitation and two-step excitation (Z-scheme reactions), as well as for direct conversion of carbon dioxide into renewable fuels using water as an electron donor. We describe the latest advances in solar water-splitting and carbon dioxide reduction systems and pathways to improve their future performance, together with challenges and solutions in their practical application and scalability, including the fixation of particulate photocatalysts, hydrogen recovery, safety design of reactor systems, and approaches to separately generate hydrogen and oxygen from water.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2023

Life cycle analysis of a hydrogen production system based on solid oxide electrolysis cells integrated with different energy and wastewater sources

Hydrogen production via water electrolysis is a promising and evolving technology. The solid oxide electrolysis cell (SOEC) is one of the several technologies for this purpose. They are alternatives to the traditional hydrogen production from fossil fuels to enhance global energy decarbonization. However, in the bid for sustainability and a green economy, these technologies are not free from causing some environmental burdens. Using life cycle assessment (LCA), the greenhouse gas emission and degree of environmental impacts by these technologies can be identified and measured throughout their lifespan. This study addresses how to quantify these CO 2 emission impacts for an electrolytic system with different energy sources. The LCA of a novel integrated hydrogen production SOEC system with energy from solar photovoltaic and bituminous powerplant is performed using simaPro, the leading global LCA solution software. Measuring the environmental impact of the electrolytic operation in terms of weight, the bituminous powerplant poses damage which is, on average 700% more than solar PV. The thermal-to-hydrogen efficiency of the SOEC system is 56%, and a probable 28% reduction in carbon footprint with heat integration. The steam generation and the manufacturing of the SOEC have a very high environmental impact potential on the system. Here, we recommend LCA and net energy analysis is carried out for every new hydrogen technology and adequate comparison to enhance sustainable and green economy.

08 HYDROGEN↗

DOE OSTI2023

Assessing feasible H2–CO2 sources in the US as Feedstocks for Sustainable Aviation Fuel Precursors: Acetic Acid and Ethanol Production via Hydrogenotrophic Pathways

The environmental impact of carbon dioxide emissions is significant, and research is focused on mitigating these emissions and developing eco-friendly technologies in line with green chemistry principles. Waste-to-energy technologies play a crucial role in converting waste into renewable energy and valuable biofuels and bioproducts. This study specifically explores the utilization of waste gas emissions, particularly carbon dioxide, from various sources in the United States for the production of sustainable aviation fuel (SAF) precursors, such as ethanol and acetic acid. The study categorizes and quantifies the volumes of carbon dioxide emissions into three types: non-biogenic, biogenic, and biogenic emissions from ethanol production facilities. Stoichiometric calculations are applied to compare the amounts of carbon dioxide from each category with the available hydrogen production capacity, determining if sufficient hydrogen is present for converting carbon dioxide into SAF precursors. The study reveals two key findings. Firstly, there is a significant reserve of carbon dioxide, approximately 1648 million metric tons per year (MMTy), combining all three categories, which would require a substantial increase of approximately 35–40 times in the existing hydrogen production capacity of 4.988 MMTy. This increased hydrogen production has the potential to yield approximately 1067.82 MMTy of acetic acid and 189.19 MMTy of ethanol annually. Secondly, upon analyzing the quality and application of the three sources of carbon dioxide with the currently available hydrogen production capacity, it is found that biogenic carbon dioxide from ethanol plants is the most suitable choice for immediate production of SAF precursors. This would theoretically result in an annual production of 1.36 MMTy of ethanol and 1.772 MMTy of acetic acid. The other two sources of carbon dioxide can be considered potential reserves for future utilization when additional hydrogen production facilities are established. The study provides a foundation for assessing the aggregation potential required for acetic acid and ethanol production. By optimizing the use of waste gases as raw materials, the study not only enables the production of SAF precursors but also contributes to the passive reduction of greenhouse gas emissions.

Carbon Dioxide↗

DOE OSTI2024

Low-Temperature Molten Salt Electrochemical CO 2 Upcycling for Advanced Energy Materials

One strategy for addressing the climate crisis caused by CO 2 emissions is to efficiently convert CO 2 to advanced materials suited for green and clean energy technology applications. Porous carbon is widely used as an advanced energy storage material because of its enhanced energy storage capabilities as an anode. Herein, we report electrochemical CO 2 upcycling to solid carbon with a controlled microstructure and porosity in a ternary molten carbonate melt at 450 °C. Controlling the electrochemical parameters (voltage, temperature, cathode material) enabled the conversion of CO 2 to porous carbon with a tunable morphology and porosity for the first time at such a low temperature. Additionally, a well-controlled morphology and porosity are beneficial for reversible energy storage. In fact, these carbon materials delivered high specific capacity, stable cycling performances, and exceptional rate capability even under extremely fast charging conditions when integrated as an anode in lithium-ion batteries (LIBs). In conclusion, the present approach not only demonstrated efficient upcycling of CO 2 into porous carbon suitable for enhanced energy storage but can also contribute to a clean and green energy technology that can reduce carbon emissions to achieve sustainable energy goals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Characterization and automated optimization of laser-driven proton beams from converging liquid sheet jet targets

Compact, stable, and versatile laser-driven ion sources hold great promise for applications ranging from medicine to materials science and fundamental physics. While single-shot sources have demonstrated favorable beam properties, including the peak fluxes necessary for several applications, high-repetition-rate operation will be necessary to generate and sustain the high average flux needed for many of the most exciting applications of laser-driven ion sources. Further, to navigate through the high-dimensional space of laser and target parameters toward experimental optima, it is essential to develop ion acceleration platforms compatible with machine learning techniques and capable of autonomous real-time optimization. Here, we present a multi-Hz ion acceleration platform employing a liquid sheet jet target. We characterize the laser-plasma interaction and the laser-driven proton beam across a variety of key parameters governing the interaction using an extensive suite of online diagnostics. We also demonstrate real-time, closed-loop optimization of the ion beam maximum energy by tuning the laser wave front using a Bayesian optimization scheme. This approach increased the maximum proton energy by 11% compared to a manually optimized wave front by enhancing the energy concentration within the laser focal spot, demonstrating the potential for closed-loop optimization schemes to tune future ion accelerators for robust high-repetition-rate operation.

Glenn, G. D. [SLAC National Accelerator Laboratory↗

DOE OSTI2023

Glass and a carbon‐free United States: What is glass's role in the upcoming green revolution?

Abstract The climate is changing rapidly due to anthropogenic greenhouse gases. Glass is a significant contributor to these emissions, with 95 million tons of CO 2 being emitted due to glass manufacturing in recent years. Furthermore, glass recycling remains poor in the United States, and most glass is left to landfill after a single use. The lack of recycling and the carbon footprint of manufacturing have made glass an environmentally damaging material despite its theoretical infinite recyclability. Additionally, glass has the potential to enable next‐generation energy materials, enabling the necessary technology for a green economy. In this review, we briefly cover the challenges of glass manufacturing and how to make glass the benchmark material for a carbon‐neutral economy.

Wilkinson, Collin↗

DOE OSTI2024

The potential of carbon markets to accelerate green infrastructure based water quality trading

Green infrastructure solutions can improve in-stream water quality in lieu of building electricity-consuming gray infrastructure. Permitted under the United States Clean Water Act, these programs allow regulated utilities to trade point-source water quality obligations with non-point source mitigation efforts in the watershed. Carbon financing can provide an incentive for water quality trading. Here we combine data on impaired waters, treatment technologies, and life cycle greenhouse gas emissions in the Contiguous United States, and compare traditional treatment technologies to alternative green infrastructure. We find green infrastructure could save $\$15.6$ billion dollars, 21.2 terawatt-hours of electricity, and 29.8 million tonnes of carbon dioxide equivalent emissions per year while sequestering over 4.2 million tonnes CO2e per year over a 40 year time horizon. Green infrastructure solutions may have the potential to generate $\$679$ million annually in carbon credit revenue (at $\$20$ per credit), which represents a unique opportunity to help accelerate water quality trading.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2024

Environmental and economic analyses of chemical recycling via dissolution of waste polyethylene terephthalate

Globally, more than 1000 organizations and 175 nations are facing the plastic waste problem and have realized the need to transition from “linear-to-circular” economy of plastics. While the current mechanical recycling technologies for plastics are struggling to increase the U.S. plastic recycling rates beyond 9%, chemical recycling technologies become important complementary technologies to the predominant mechanical recycling that are needed to realize the circular economy in plastics supply chains. Dissolution is one such chemical recycling technology that can recycle waste plastic back into high-quality virgin grade plastic. However, the environmental and economic impacts of chemical recycling of waste polyethylene terephthalate (PET) via dissolution technology using a green solvent are unknown. Our study evaluated environmental metrics such as greenhouse gas (GHG) emissions and cumulative energy demand, and economic metrics such as net present value (NPV), minimum selling price, payback period, return on investment, and discounted internal rate of return for three dissolution processes with polymer recovery via anti-solvent, evaporation, and cooling precipitation techniques. The dissolution process with evaporation technique was the most economically favorable, whereas that with cooling technique was the most environmentally favorable. The anti-solvent approach had low economic performance and the highest environmental impacts. The NPV for all of these technologies ranged from $2.67 MM to $10.93 MM for a capacity of 8,400 MT/year and was found to be the highest for dissolution with evaporation approach and the least for anti-solvent approach. The cradle-to-gate GHG emissions and energy demand for PET dissolution processes ranged from 1.33-3.77 kg CO2-eq/kg of chemically recycled (CR) PET and18.9-56.1 MJ/kg of CR-PET, respectively. These economic and environmental metrics will be helpful in evaluating the sustainability of circular PET supply chains in the U.S.

09 BIOMASS FUELS↗

DOE OSTI2025

Leaky ribosomal scanning enables tunable translation of bicistronic ORFs in green algae

Advances in sequencing technology have unveiled examples of nucleus-encoded polycistrons, once considered rare. Exclusively polycistronic transcripts are prevalent in green algae, although the mechanism by which multiple polypeptides are translated from a single transcript is unknown. Here, we used bioinformatic and in vivo mutational analyses to evaluate competing mechanistic models for translation of bicistronic mRNAs in green algae. High-confidence manually curated datasets of bicistronic loci from two divergent green algae, Chlamydomonas reinhardtii and Auxenochlorella protothecoides, revealed a preference for weak Kozak-like sequences for ORF 1 and an underrepresentation of potential initiation codons before the ORF 2 start codon, which are suitable conditions for leaky ribosome scanning to allow ORF 2 translation. We used mutational analysis in A. protothecoides to test the mechanism. In vivo manipulation of the ORF 1 Kozak-like sequence and start codon altered reporter expression at ORF 2, with a weaker Kozak-like sequence enhancing expression and a stronger one diminishing it. A synthetic bicistronic dual reporter demonstrated inversely adjustable activity of green fluorescent protein expressed from ORF 1 and luciferase from ORF 2, depending on the strength of the ORF 1 Kozak-like sequence. Our findings demonstrate that translation of multiple ORFs in green algal bicistronic transcripts is consistent with episodic leaky scanning of ORF 1 to allow translation at ORF 2. This work has implications for the potential functionality of upstream open reading frames (uORFs) found across eukaryotic genomes and for transgene expression in synthetic biology applications.

59 BASIC BIOLOGICAL SCIENCES↗