bluuebunny/crossref_metadata_2025_split huggingface dataset:
Electrosynthesis of Glyoxylic Acid By Electrochemical Reduction of Oxalic Acid and Oxidation of Glyoxal inside Co-Laminar Flow Cells
Authors: Mirzaie Farzad , Goulet Marc-Antoni 
Published: August 2024

This study investigates the simultaneous electrosynthesis of glyoxylic acid through electrochemical reduction of oxalic acid and oxidation of glyoxal inside a co-laminar flow reactor. This system offers specific advantages over traditional beaker cells including: continuous operation and controlled mixing of products.
This study involves a systematic exploration of operating conditions such as flow rate, applied potential, current density, electrode gap and influence of specific electrocatalysts. These operating conditions are varied while the yield and current efficiency of the cell are measured. In this way, the optimum conditions for electrosynthesis of glyoxylic acid are determined and insight into the efficiency of other electrosynthesis reactions is obtained.
Metal-Organic Framework-Based Materials for Heavy Metal Sensing in Aqueous Media
Authors: Šljukić Biljana , Milikić Jadranka , Radinović Kristina , Savić Marjetka , Janošević Ležaić Aleksandra , Ćirić-Marjanović Gordana 
Published: August 2024

Industrial development leads to an increasing amount of pollutants including heavy metal ions in surface and subsurface waters. For instance, wastewater from battery manufacturing, paint manufacturing or metal plating, contain heavy metals in high concentrations. The heavy metals are typically non-biodegradable and not-easy to excrete. Their presence within the organisms causes damage and failure of different organs. Consequently, the permissible concentrations of heavy metal ions in drinking water set by the World Health Organization are on a ppb level.
In this work, electrode materials based on metal-organic frameworks (MOFs) are prepared and studied for sensing of heavy metals in aqueous media. These involved MOFs in their pristine form, composites of pristine MOFs and conducting polymer polyaniline as well as their carbonized derivatives. Cadmium and lead ions were used as model pollutants. Thorough physico-chemical characterization of the prepared materials was done using scanning electron microscopy, Raman spectroscopy, and dynamic light scattering. Electroanalytical performance was scrutinized using anodic stripping voltammetry and correlated with materials’ structural, morphology and textural properties. Limits of detection and sensitivity were determined upon optimization of the experimental conditions to identify the best material. Moreover, materials proved to be suitable for two heavy metal ions sensing in real river samples.

Acknowledgments

This work was supported by the Science Fund of the Republic of Serbia, grant number 7750219, Advanced Conducting Polymer-Based Materials for Electrochemical Energy Conversion and Storage, Sensors and Environmental Protection-AdConPolyMat (IDEAS programme).
Light-Induced Redox Dynamics in Plasmonic Nanostructures and Photosensitizer Transition Metal Compounds
Authors: Sprague-Klein Emily 
Published: August 2024

Solar energy harvesting is a nuanced scientific field that involves precise control across energy, time, and nanometer length scales. The understanding of how to harness sunlight to promote chemical reactions is vital for the advancement of renewable energy applications and a sustainable future. Limited knowledge of the precise chemical mechanisms underlying solar energy harvesting restricts widespread technological use and the development of photovoltaic devices that utilize light-harvesting biodegradable materials. My research focuses on developing a fundamental understanding of visible light-activated excited state chemistry that is of great importance in elucidating the mechanisms, structures, and design features for catalysis. In this talk, we will examine excited-state chemical structure dynamics in nanomaterials that use light-matter interactions to drive interfacial or intramolecular charge transfer. Steady-state and time-resolved optical/X-ray spectroscopy allow for the observation of these dynamics across an expansive timescale—from the seconds timescale of oxygen-evolving reactions to the ultrafast timescales of electronic and vibrational motion. Novel light-matter interactions in plasmonic nanostructures, biomimetic metal oxides, and molecular transition metal complexes will be discussed. The talk will conclude with future opportunities for expanding the scope of nanoscale photocatalysis and for designing enhanced localized control over excited-state chemistry.
[1] E. A. Sprague-Klein*, X. He, M. W. Mara, B. J. Reinhart, S. Lee, L. M. Utschig, K. L. Mulfort, L. X. Chen*, D. M. Tiede*. “Photo-Electrochemical Effect in the Water Oxidation Catalyst Cobalt-Phosphate (CoPi),” ACS Energy Letters, 2022, 7, 9, 3129–3138.
[2] N. L. Warren, U. Yunusa, A. B. Singhal, E. A. Sprague-Klein*. "Facilitating Excited-State Plasmonics and Photochemical Reaction Dynamics," Chemical Physics Reviews, (Accepted December 2023).
[3] U. Yunusa, N. Warren, D. Schauer, P. Srivastava, E. Sprague-Klein*. "Plasmon resonance dynamics and enhancement effects in Tris(bipyridine)ruthenium(II) gold nanosphere oligomers," Nanoscale, (Under Review).
(Invited) Insights into Atomistic Processes at Electrified Solid/Liquid Interfaces from Ab Initio Calculations
Authors: Todorova Mira , Yang Jing , Surendralal Sudarsan , Yoo Suhyun , Deissenbeck Florian , Wippermann Stefan , Neugebauer Joerg 
Published: August 2024

Many of the challenges we face today towards achieving a greener economy focus on processes occurring at electrified solid/liquid interfaces. Understanding how the interactions between the solid, the liquid and dissolved species are affected by the applied potential will aid our ability to achieve rational design and targeted optimization of relevant processes. Hereby, ab initio molecular dynamic simulations including explicit modelling of the aqueous environment have proven an indispensable tool to gain insights into reaction mechanisms. More approximate choices to modelling the electrolyte, such as implicit solvent models, are however also popular. The talk will discuss the suitability of approximate models for the aqueous environment to study, e.g., the stability of surface phases in the Mg/H2O system and incorporation of impurities in nano-aerogels during synthesis [1,2], by coupling DFT calculations with thermodynamic models. Furthermore, insights into reaction mechanism at electrified solid/liquid interfaces enabled by our recent developments of a thermopotentiostat [3,4] will be presented, using the example of Pt[5].
[1] S.-H. Kim, S.-H. Yoo, S. Shin, A. El-Zoka, O. Kasian, J. Lim, J. Jeong, C. Scheu, J. Neugebauer, H. Lee, M. Todorova, B. Gault, Adv. Mater. 34, 2203030 (2022)
[2] S.-H. Kim, S.-H. Yoo, P. Chakraborty, J. Jeong, J. Lim, A. El-Zoka, L. Stephenson, T. Hickel, J. Neugebauer, C. Scheu, M. Todorova, B. Gault, J. Am. Chem. Soc. 144, 987 (2022)
[3] S. Surendralal, M. Todorova, M. Finnis, and J. Neugebauer, Phys. Rev. Lett. 120, 246801 (2018)
[4] F. Deißenbeck, C. Freysoldt, M. Todorova, J. Neugebauer, and S. Wippermann, Phys. Rev. Lett. 126, 136803 (2021)
[5] S. Surendralal, M. Todorova, and J. Neugebauer, Phys. Rev. Lett. 126,166802 (2021)
(Invited) Battery Manufacturing Needs from the Perspective of DOE's Advanced Materials and Manufacturing Technologies Office
Authors: Suh Changwon 
Published: August 2024

The Department of Energy’s Advanced Materials and Manufacturing Technologies Office (AMMTO) continues to invest in energy storage research, development, and demonstration (RD&D) to help stakeholders improve efficiency, cut costs, and make materials, components, and systems with superior performance. Despite recent promising advances, manufacturing capabilities are still necessary to meet the expected demand for batteries as we move toward a clean energy economy. Strengthening the domestic manufacturing supply chains is also another important task to pursue in parallel. A multi-pronged approach is required to strengthen domestic battery manufacturing and reduce time to commercialization and deployment of transformative technologies. AMMTO recognizes a number of unmet needs that need to be addressed including development of manufacturing processes and equipment that take advantage of the most recent technical advances as well as effective utilization of data-driven analysis and experimentation to assist in manufacturing optimization.
In this talk, AMMTO’s perspective on energy storage technology development and manufacturing will be discussed, highlighting current gaps and challenges that need to be addressed. In addition, there will be a robust discussion of a wide variety of DOE’s efforts in the context of technical and manufacturing challenges regarding scale-up and performance that still prevent the electrochemical energy storage community from achieving cost targets and commercial viability.
(Invited) Single Crystal Ni-Rich Cathode Materials: Synthesis, Scaleup and Validation
Authors: Xiao Jie 
Published: August 2024

Synthesis of high-performance single crystal Ni-rich NMC, especially when Ni≥0.8, poses a challenge. A conflict exists because as Ni content increase in NMC811, a lower calcination temperature is preferred due to Ni reduction at elevated temperatures, while high temperatures favour single crystal growth.Therefore, molten salt is sometimes employed as the reaction media to promote growth of single crystal NMC811. In general, four approaches for synthesizing of Ni-rich NMC single crystals: molten salt, hydrothermal, direct solid-state synthesis and multi-step lithiation. Molten salt and hydrothermal approaches result in the formation of well-segregated large crystals, but they also increase manufacturing cost. Direct solid-state synthesis, which involves ball milling all precursors together followed by calcination, is a time-saving approach. However, it poses challenge for impurity control due to contamination from milling media, and it can damage the material structure. The calcination of TM(OH)2 precursor with LiOH at very high sintering temperatures forms micron-sized primary particles which, however, still exhibit significantly agglomerated. A post-synthesis milling process is required to break down those NMC811 crystal clusters.
This talk will discuss an innovative nanoscale phase separation approach for synthesis of high-performance single crystal NMC811 that is readily adaptable for industry manufacturing. The reaction mechanism of single crystal growth is investigated to understand the synthesis-morphology-performance relationship in growing single crystal NMC811 in the absence of molten salts. The scaled single crystal NMC811 is then further validated in a 2Ah Li-ion pouch cells, demonstrating 1000 stable cycling, confirming the feasibility of this new synthesis approach. This work provides new insights that are broadly applicable for cost-efficient large-scale synthesis of single crystals for different advanced battery technologies to accelerate deep decarbonization process.
Strategies for Printing Ultra-Thin and Variable Width Lithium Foil
Authors: Cabaniss Joseph Emory , Gao Yuqi , Yakovleva Marina 
Published: August 2024

The commercial success of rechargeable lithium-related batteries in electronic devices since the 1990s has been remarkable. Technologies in the field continue to develop to make batteries safer, longer lasting, and more powerful. Emerging lithium-ion battery technologies such as solid-state batteries or high-silicon anode materials utilize, for example, ultra-thin lithium metal foil due to lithium metal high specific capacity (3860 mA h g-1), however; traditional thin lithium foil manufacturing methods have proven challenging at scale due to metal reactivity, poor foil tensile strength, and safety concerns. Additionally, lithium metal foil is needed in a variety of thicknesses, widths, and surface characteristics, which are all crucial for advancing lithium metal based batteries. Fortunately, it can be done via industry standard technologies when using LIOVIX®, Printable Lithium Technology.
LIOVIX formulation has been coated using direct slot die technology at the benchtop scale and tension web slot die technology at the Roll-to-Roll (R2R) scale. Slot die technology facilitates two major elements of this process; particles larger than the theoretical wet film thickness can be deposited, and also the material can be shipped, delivered, and mixed without exposing lithium to air until it leaves the slot die head. This approach allowed us to achieve a uniform coating with heights ranging from 7 µm to 30 µm at a variety of coating widths. This has been done at the benchtop level at speeds up to 200 mm s-1 while maintaining a uniform coating on a copper substrate. R2R coating has done via a tension web coater, with similar theoretical wet film thickness. Specifically, the application of LIOVIX as a coating is particularly noteworthy for offering a strategic advantage in large scale manufacturing while maximizing the electrochemical performance.
LIOVIX formulation enables the R2R production of lithium foil materials, and using a pre-metering system, the coating can be reliably produced at a variety of areal capacity targets.
Scaling and Commercializing Continuous Supercritical Hydrothermal Single Crystal Cathode Active Material Manufacturing
Authors: Lim Jin , Shin Youngho 
Published: August 2024

Current polycrystalline cathode active materials (CAMs) in the market face a significant challenge during charge-discharge cycles. The lithiation and de-lithiation processes induce volume changes within the CAMs, leading to strain along grain boundaries. This strain, arising from the expansion of crystals in different orientations, often results in material pulverization, creating void fractions. Such deterioration leads to increased impedance, capacity degradation, and shorter cycle life.
Addressing these challenges, there is an emerging demand for single crystal (SC) CAMs, which promise enhanced performance by eliminating internal void fractions and grain boundaries. The continuous supercritical hydrothermal process, invented at Argonne National Laboratory, offers an innovative and cost-effective method to produce SC CAMs. This method effectively reduces energy consumption and production costs, while also lowering carbon emissions.
In this presentation, we provide a comprehensive overview of the advancements in scaling up and commercializing continuous supercritical hydrothermal process for SC CAM manufacturing. Our focus is on the efforts undertaken by ACT-ion Battery Technologies, the industry commercialization partner, highlighting the significant strides made towards implementing this promising solution on a practical level.
Bridging the Gap: Scaling up Processes for the Development of Li-Rich Mn-Rich Layered Oxides
Authors: Siu Carrie , Zuba Mateusz , Buyuker Isiksu , Kahvecioglu Ozgenur 
Published: August 2024

As the global demand for more powerful and long-lasting energy storage solutions continues to grow, Li-rich Mn-rich layered oxides (LMR) emerges as a promising class of next-generation cathode materials for lithium-ion batteries. The LMR material stands out due to its impressive electrochemical specific capacity, surpassing 280 mAh g–1, along with a high discharge voltage exceeding 3.5 V. It also boasts a remarkable specific energy density close to 1000 Wh kg–1, all while maintaining a relatively lower cost.
Current synthesis methods often rely on batch coprecipitation reactions followed by the calcination of precipitated Mn-rich precursors. However, the inherent challenges of batch reactions, particularly in terms of reproducibility and quality, prompt the exploration of more sophisticated approaches. Moreover, the transition from benchtop experiments to large-scale production introduces a distinct set of challenges. Parameters that work seamlessly on a smaller scale may not translate as effectively when producing the material at the kilogram scale. This scaling-up process involves navigating complexities such as chemical handling risks, and challenges related to reaction heat transfer and mixing efficiency. These factors collectively underscore the difficulties in achieving precise control over critical precursor characteristics, including primary and secondary particle size, morphology, tap density, and stoichiometry.
In response to these challenges, this presentation will discuss an innovative approach. High-quality Li-rich Mn-rich materials are synthesized using continuous coprecipitation, facilitated by a pre-pilot scale Taylor Vortex Reactor (TVR) at the Materials Engineering Research Facility (MERF) in Argonne National Lab (ANL). This emerging synthesis technology offers a scalable solution for the production of high-quality cathode materials. This presentation will delve into the intricacies of the synthesis process, providing valuable insights into the relationship between the characteristics of the synthesized LMR precursors and their subsequent impact on cathode performance.
Revealing the Effects of Polymer Additives on Zn Dendrite Suppression in Aqueous Zn Batteries via in-Situ EC-AFM
Authors: Xia Ying , Tao Jinhui , Du Jingshan , Shi Chenyang , Sun Hae Ra Shin , Zhang Mingyi , Orme Christine , Kaiser Mitchell , Thallapally Praveen K , Sushko Maria , De Yoreo James J , Liu Jun 
Published: August 2024

Polyethylene glycol (PEO) is a commonly used polymer in the field of batteries for achieving flat and uniform electrodes to enhance the performance of batteries, such as lithium batteries and zinc (Zn) batteries. However, the impact of PEO on the electrochemical deposition of Zn metal on electrodes remains uncertain. In this study, we selected ZnSO4 solution as electrolyte and copper (Cu) substrates as electrodes, which are widely applied in Zn batteries. We used in situ electrochemical atomic force microscopy (EC-AFM) to observe the nucleation and growth of Zn metal plates on the Cu substrate in the presence of different concentrations of ZnSO4 and PEO additives. Our results indicate that PEO biases the crystallographic orientation of the initially deposited Zn metal nuclei, but does not have an obvious influence on subsequent growth. Based on our findings, we hypothesize that PEO primarily interacts with the Cu substrate to adjust the interfacial energy of the Cu-electrolyte interfaces. In contrast, due to the lack of apparent change in the Zn growth rate, we postulate that PEO does not affect the delivery rate of Zn2+ to the electrode surface. The consistent aspect ratio of the Zn plates combined with the lack of an effect on growth rates further suggests that PEO does not interact significantly with the surface of the newly formed Zn plates. The Zn metal will undergo surface reorganization in a mildly acidic aqueous solution as a result of oxidation of Zn, which is not affected by PEO adsorption. Our findings provide both insight into the underlying mechanism by which PEO promotes electrode flattening in Zn batteries and a standardized protocol for elucidating the impact of additives on the morphological evolution of interfaces during electrochemical deposition.
Work by C.O. was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.
Making Nanoporous Metals By Electrochemical Etching without Sacrificing Metals
Authors: Ng Alexander , Koh Hyeongjun , Detsi Eric 
Published: August 2024

The creation of nanoporous metals typically involves selective etching of a less noble material from a parent alloy, leaving the etched metal as a waste product. As we aim to achieve a circular economy, recent studies have proposed more sustainable methods to recover some of the sacrificial metals that are lost during the nanoporous metal fabrication process. However, even with these new methods, we still lose up to 35 atomic percent of the sacrificial metal.[1] In this presentation, I will introduce an innovative electrochemical method for creating nanoporous metals that almost entirely eliminates the loss of any sacrificial metals during fabrication. By combining and modifying the etching approach of “reduction-induced decomposition”, introduced in [2],and “electrochemical plating-stripping for nanoporous structures”, introduced in [3], we can create nanoporous metals without losing sacrificial materials. During my presentation, I will demonstrate how a dense silver thin film can be transformed into a fully nanoporous structure through electrochemical plating and reduction. The innovation is that we can create these nanoporous structures by reversibly utilizing ions present in the electrolyte, without consuming them in the reaction. I will also discuss ways to tune the structure size and introduce hierarchical porous morphology in the process. Electrochemistry data, microscopy, and X-ray scattering are used to confirm the porosity and structure size in the sample. Furthermore, in this talk, I will demonstrate the broad generalization of this technique, by showing how we have extended this novel technique to bimetallic alloys to create composite nanoporous metals, consisting of layered dissimilar nanoporous metals.
References
[1] J.S. Corsi, J. Fu, L. Wang, S.S. Welborn, Z. Wang, E. Detsi, Sacrificial Silver Recovery during Nanoporous Gold Formation by Electrolytic Dealloying of Gold-Silver Alloy, J. Electrochem. Soc. 169 (2022) 063501. https://doi.org/10.1149/1945-7111/ac6344.
[2] C. Wang, Q. Chen, Reduction-Induced Decomposition: Spontaneous Formation of Monolithic Nanoporous Metals of Tunable Structural Hierarchy and Porosity, Chem. Mater. 30 (2018) 3894–3900. https://doi.org/10.1021/acs.chemmater.8b01431.
[3] X. Jin, J. Lu, P. Liu, H. Tong, The electrochemical formation and reduction of a thick AgCl deposition layer on a silver substrate, Journal of Electroanalytical Chemistry. 542 (2003) 85–96. https://doi.org/10.1016/S0022-0728(02)01474-2.