Claus Daniel

Electrification to reduce or eliminate greenhouse gas emissions is essential to mitigate climate change. However, a substantial portion of our manufacturing and transportation infrastructure will be difficult to electrify and/or will continue to use carbon as a key component, including areas in aviation, heavy-duty and marine transportation, and the chemical industry. In this Roadmap, we explore how multidisciplinary approaches will enable us to close the carbon cycle and create a circular economy by defossilizing these difficult-to-electrify areas and those that will continue to need carbon. We discuss two approaches for this: developing carbon alternatives and improving our ability to reuse carbon, enabled by separations. Furthermore, we posit that co-design and use-driven fundamental science are essential to reach aggressive greenhouse gas reduction targets.

R2R processing is used to manufacture a wide range of products for various applications which span many industrial business sectors. The overall R2R methodology has been in use for decades and this continuous technique traditionally involves deposition of material(s) onto moving webs, carriers or other continuous belt-fed or conveyor-based processes that enable successive steps to build a final version which serves to support the deposited materials. Established methods that typify R2R processing include tape casting, silk-screen printing, reel-to-reel vacuum deposition/coating, and R2R lithography. Products supported by R2R manufacturing include micro-electronics, electro-chromic window films, PVs, fuel cells for energy conversion, battery electrodes for energy storage, and barrier and membrane materials. Due to innovation in materials and process equipment, high-quality yet very low-cost multilayer technologies have the potential to be manufactured on a very cost-competitive basis. To move energy-related products from high-cost niche applications to the commercial sector, the means must be available to enable manufacture of these products in a cost-competitive manner that is affordable. Fortunately, products such as fuel cells, thin- and mid-film PVs, batteries, electrochromic and piezoelectric films, water separation membranes, and other energy saving technologies readily lend themselves to manufacture using R2R approaches. However, more early-stage research ismore » needed to solve the challenge of linking the materials (particles, polymers, solvents, additives) used in ink and slurry formulations and the coating and drying processes to the ultimate performance of the final R2R product, especially for a process that uses multiple layers of deposition to achieve the end product.To solve the problems associated with these challenges, the R2R Collaboration is executing a research program with outcomes that will ultimately link modeling, processing, metrology and defect detection tools, thereby directly relating the properties of constituent particles and processing conditions to the performance of final devices. The Collaboration team and their research efforts with industry involvement are illustrated schematically in Figure 1. This collaborative approach was designed to foster identification and development of materials and processes related to R2R for clean-energy materials development. Using computational and experimental capabilities by acknowledged subject matter experts within the supported National Laboratory system, this project leverages the capabilities and expertise at each of five National Laboratories to further the development of multilayer technologies that will enable high-volume, cost-competitive platforms. Figure 1. The R2R AMM DOE Laboratory Collaboration team and major research efforts. Source: ORNLA typical R2R process has three steps: (1) mixing of particles and various constituents in a slurry, (2) coating of the ink/slurry mixture on a substrate, and (3) drying/curing and processing of the coating. Final performance of devices made via R2R processes is dependent on the active materials (e.g., electrochemical particles in battery or fuel cell electrodes) and the device structure that stems from the governing component interactions within the various steps. However, a fundamental understanding of the underlying mechanisms and phenomena is still lacking, which is why industrial-scale R2R process development and manufacturing is still largely empirical in nature.The FY 2019 through FY 2021 program addresses aspects of the following two targets from the AMO Multi-Year Program Plan: •Target 8.1 Develop technologies to reduce the cost per manufactured throughput of continuous R2R manufacturing processes.oIncreasing throughput of R2R processes by 5 times for batteries (to 50 square feet per minute (50 ft2/min)) and capacitors and 10 times for printed electronics and the manufacture of other substrates and MEs used in support of these products.oDeveloping resolution capabilities to enable registration and alignment that will detect, align, and co-deposit multiple layers of coatings and print < 1-micron (1 µm) features using continuous process scalable for commercial production.oDeveloping scalable and reliable R2R processes for solution deposition of ultra-thin (<10 nm) films for active and passive materials. oDevelop in-line multilayer coating technology on thin films with yields greater than 95%.•Target 8.2 Develop in-line instrumentation tools that will evaluate the quality of single and multilayer materials in-process.oDeveloping in-line QC technologies and methodologies for real-time identification of defects and expected product properties “in-use/application” during continuous processing at all size-scales with a focus on the “micro” and “nano” scale traces, lines, and devicesoDeveloping technologies to increase the measurement frequency of surface rheology without significant cost incr « less

The U.S. Department of Energy's Office of Scientific and Technical Information

Metal oxide coatings have been reported to be an effective approach for stabilizing cathode interfaces, but the associated chemistry is unclear. In this work, thin films of TiO₂, ZnO, and Cr₂O₃, which have different surface acidities/basicities, were used to modify the surface chemistry of LiNi_0.6Mn_0.2Co_0.2O₂ and study the acidity’s role in the cathode/electrolyte interphase composition and impedance under high-voltage cycling (4.5 V vs Li/Li⁺). Cathodes with more acidic surfaces provided higher initial specific capacity and capacity retention with cycling. More basic surfaces had higher initial impedance and greater impedance growth with cycling. These differences appeared to depend on the degree of LiPF₆ salt decomposition at the interface, which was related to acidity, with more neutral surfaces having a LiF/Li_xPO_yF_z ratio close to unity, but basic surfaces had substantially more LiF. This chemistry was more significant than the cathode electrolyte interphase (CEI) thickness as the more acidic surfaces formed a thicker CEI than the basic surface, resulting in better capacity retention. These results suggest that the Brønsted acidity of cathodes directly influences electrolyte degradation, ion transport, and thus, cell lifetime.

R2R processing is used to manufacture a wide range of products for various applications which span many industrial business sectors. The overall R2R methodology has been in use for decades and this continuous technique traditionally involves deposition of material(s) onto moving webs, carriers or other continuous belt-fed or conveyor-based processes that enable successive steps to build a final version which serves to support the deposited materials. Established methods that typify R2R include tape casting, silk-screen printing, reel-to-reel vacuum deposition/coating and R2R lithography. Products supported by R2R manufacturing include micro-electronics, electro-chromic window films, PVs, fuel cells for energy conversion, battery electrodes for energy storage, and barrier and membrane materials. Due to innovation in materials and process equipment, high-quality yet very low-cost multilayer technologies have the potential to be manufactured on a very cost-competitive basis. To move energy-related products from high-cost niche applications to the commercial sector, a means must be available to enable manufacture of these products in a cost-competitive manner that is affordable. Fortunately, products such as fuel cells, thin- and mid-film PVs, batteries, electrochromic and piezoelectric films, water separation membranes, and other energy saving technologies readily lend themselves to manufacture using R2R approaches. However, more early-stage research is neededmore » to solve the challenge of linking the materials (particles, polymers, solvents, additives) used in ink and slurry formulations, though the ink processing, coating and drying processes, to the ultimate performance of the final R2R product, especially for a process that uses multiple layers of deposition to achieve the end product.To solve the problems associated with this R2R “Grand Challenge”, the R2R AMM DOE Laboratory Collaboration is executing a research program with outcomes that will ultimately link modeling, processing, metrology and defect detection tools, thereby directly relating the properties of constituent particles and processing conditions to the performance of final devices. The Collaboration team and their research efforts with industry involvement are illustrated schematically in Figure 1. This collaborative approach was designed to foster identification and development of materials and processes related to R2R for clean-energy materials development. Using computational and experimental capabilities by acknowledged subject matter experts within the supported National Laboratory system, this project leverages the capabilities and expertise at each of five national laboratories to further the development of multilayer technologies that will enable high-volume, cost-competitive platforms.Figure 1 The R2R AMM DOE Laboratory Collaboration team and major research efforts. Source: ORNLA typical R2R process has three steps: 1) mixing of particles and various constituents in a slurry, 2) coating of the ink/slurry mixture on a substrate, and 3) drying/curing and processing of the coating. Final performance of devices made via R2R processes is dependent on the active materials (e.g. electrochemical particles in battery or fuel cell electrodes) and the device structure that stems from the governing component interactions within the various steps. However, a fundamental understanding of the underlying mechanisms and phenomena is still lacking, which is why industrial-scale R2R process development and manufacturing is still largely empirical in nature.The FY 2019 through FY 2021 program addresses aspects of the following two targets from the AMO Multi-Year Program Plan: •Target 8.1 Develop technologies to reduce the cost per manufactured throughput of continuous R2R manufacturing processes.oIncreasing throughput of R2R processes by 5 times for batteries (to 50 square feet per minute (50 ft2/min)) and capacitors and 10 times for printed electronics and the manufacture of other substrates and MEs used in support of these products.oDeveloping resolution capabilities to enable registration and alignment that will detect, align, and co-deposit multiple layers of coatings and print < 1-micron (1 µm) features using continuous process scalable for commercial production.oDeveloping scalable and reliable R2R processes for solution deposition of ultra-thin (<10 nm) films for active and passive materials. oDevelop in-line multilayer coating technology on thin films with yields greater than 95%.•Target 8.2 Develop in-line instrumentation tools that will evaluate the quality of single and multilayer materials in-process.oDeveloping in-line QC technologies and methodologies for real-time identification of defects and expected product properties “in-use/application” during continuous processing at all size-scales with a focus on the “micro” and “nano” scale traces, lines, and devicesoDeveloping technologies to increase the measurement frequency of surface rheology « less