Engineering topics

Shin, Youngho

Publications and source records attributed to Shin, Youngho.

6 records

DOE OSTI2024

Understanding improved cycling and thermal stability of compositionally graded Ni-rich layered LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathode materials

The concentration gradient is a strategic design, adjusting the distribution of Ni, typically with a higher Ni content in the core and a higher Mn content toward the surface. This design leverages the pivotal role of the Ni/Mn ratio, seeking to optimize cathode performance by balancing Ni's high capacity with Mn's stabilizing effects, particularly at the surface where degradation commonly occurs during cycling. Here, our study delves into the intricate structural and chemical transformations within concentration gradient cathode materials during electrochemical cycling. Utilizing advanced synchrotron X-ray techniques, including hard and soft X-ray absorption spectroscopy (hXAS, sXAS), and nanoscale X-ray imaging, we investigate buried changes in concentration gradient LiNi 0.6 Mn 0.2 Co 0.2 O 2 (CG NMC622). Contrary to conventional assumptions, our findings challenge the notion that cycling stability relies solely on Mn stability. Unraveling the roles of Ni and Mn, we uncover how their individual and collective contributions impact the cathode's overall performance. This investigation transcends established paradigms, shedding light on the crucial mechanisms governing the enhanced cycling stability of Nirich layered cathode materials.

25 ENERGY STORAGE↗

DOE OSTI2023

High‐Nickel Heterostructured Cathodes with Local Stoichiometry Control for High‐Voltage Operation

The growing demand for lithium‐ion batteries to power electric vehicles and other energy‐dense devices continues to fuel the need for cathodes of increasingly higher nickel in cathodes. The relentless pursuit of high Ni content, however, raises concerns on compromising cell lifetime and safety, especially under high‐voltage operation. Alternative to the traditional design of uniform or core–shell composition, we report a rational control of local stoichiometry in high‐Ni cathodes, enabling their high thermal and cycling stabilities—up to 258 °C at the fully charged state and 91.4% capacity retention for 100 cycles between 2.7 and 4.4 V. Multimodal synchrotron X‐ray characterization unveils the heterostructure of secondary particles, featuring a high‐Ni core (LiNi 0.90 Mn 0.05 Co 0.05 O 2 ) covered by a thin Ni‐gradient layer that remains stable over prolonged cycling due to suppressed oxygen release and structural deterioration. This work underlines, the intricate interplay between local stoichiometry and redox reactions in stabilizing high‐Ni cathodes for high‐voltage operation while ensuring safety.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Resolution-enhanced X-ray fluorescence microscopy via deep residual networks

Abstract Multimodal hard X-ray scanning probe microscopy has been extensively used to study functional materials providing multiple contrast mechanisms. For instance, combining ptychography with X-ray fluorescence (XRF) microscopy reveals structural and chemical properties simultaneously. While ptychography can achieve diffraction-limited spatial resolution, the resolution of XRF is limited by the X-ray probe size. Here, we develop a machine learning (ML) model to overcome this problem by decoupling the impact of the X-ray probe from the XRF signal. The enhanced spatial resolution was observed for both simulated and experimental XRF data, showing superior performance over the state-of-the-art scanning XRF method with different nano-sized X-ray probes. Enhanced spatial resolutions were also observed for the accompanying XRF tomography reconstructions. Using this probe profile deconvolution with the proposed ML solution to enhance the spatial resolution of XRF microscopy will be broadly applicable across both functional materials and biological imaging with XRF and other related application areas.

36 MATERIALS SCIENCE↗

DOE OSTI2023

3D Quantification of Elemental Gradients within Heterostructured Particles of Battery Cathodes

Heterogenous architectures with elemental gradients tailored within particles have been pursued to combat the instabilities limiting Ni-rich cathode materials for lithium-ion batteries. The growth of different compositional layers is accomplished during the synthesis of hydroxide precursors. However, the extent to which these concentration gradients are modified during high-temperature reactions is difficult to establish in their intact, spherical form. Here, we show the entire three-dimensional structure of a secondary particle can be resolved nondestructively with differential X-ray absorption spectroscopy (XAS) through transmission X-ray microscopy (TXM). The relationship between particle location and elemental content was fully quantified, with high statistical significance, for heterostructures possessing different compositional gradients in the precursors with 90:5:5 Ni:Mn:Co core compositions. Reduced elemental heterogeneity was observed after high-temperature synthesis, but gradients remained. In conclusion, the methodology presented should be used to guide synthesis while assuring that gains in electrochemical performance are linked to precise elemental distributions at the nanoscale.

25 ENERGY STORAGE↗

DOE OSTI2022

Synthesis of platinum nanoparticles on strontium titanate nanocuboids via surface organometallic grafting for the catalytic hydrogenolysis of plastic waste

Pt/SrTiO 3 (Pt/STO), prepared on small scale by atomic layer deposition (ALD), is a capable heterogeneous catalyst for the selective hydrogenolysis of polyolefins to hydrocarbon oils, providing a promising approach for upcycling plastic waste. However, because deposition by ALD is costly and resource-intensive, a new synthesis of Pt/STO is needed to effectively scale catalyst production and pursue the commercialization of upcycling processes. To that effect, this work details a scalable deposition method for Pt/STO made by surface organometallic chemistry (SOMC) techniques using Pt(II) acetylacetonate or and trimethyl(methylcyclopentadienyl)platinum. The STO support was calcined (550 °C), treated with ozone (200 °C), and finally steamed (200 °C) to afford a clean STO surface populated with only hydroxyl groups. Pt precursors were dissolved in toluene and deposited onto STO. After reduction at 300 °C, the STO support was decorated with 1.0–1.5 nm Pt nanoparticles. The size and loading of these nanoparticles were varied by employing a multi-cycle deposition and oxidation and/or reduction process designed to ALD techniques. In conclusion, these Pt/STO catalysts hydrogenolyzed isotactic polypropylene into liquid products (>95% yield) with average molecular weights of 200–300 Da (~25 carbon atoms) and narrow size distributions at 300 °C and 180 psi H 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Batteries (2021 Annual Progress Report)

This document summarizes the progress of VTO battery R&D projects supported during the fiscal year 2021 (FY 2021). In FY 2021, the DOE VTO battery R&D funding was approximately $\$$115 million. Its R&D focus was on the development of high-energy batteries for EVs as well as very high-power devices for hybrid vehicles. The electrochemical energy storage roadmap (which can be found at the EERE Roadmap web page2) describes ongoing and planned efforts to develop electrochemical storage technologies for EVs. To advance battery technology, which can in turn improve market penetration of PEVs, the program investigates various battery chemistries to overcome specific technical barriers, e.g., battery cost, performance, life (both the calendar life and the cycle life), its tolerance to abusive conditions, and its recyclability/sustainability. VTO R&D has had considerable success, lowering the cost of EV battery packs to $\$$185/kWh in 2019 (representing more than 80% reduction since 2008) yet even further cost reduction is necessary for EVs to achieve head-to-head cost competitiveness with ICEs (without Federal subsidies). In addition, today’s batteries also need improvements in such areas as their ability to accept charging at a high rate, referred to as extreme fast charging (XFC) (15 minute charge) – to provide a “refueling” convenience similar to ICEs, and the ability to operate adequately at low temperatures. Research into “next-gen lithium-ion” batteries which would provide such functionalities is one of the R&D focus areas. VTO is funding research on both “next gen” chemistries (which employ an alloy anode and/or a high voltage cathode) and beyond lithium-ion (BLI) chemistries (which can, for example, employ a lithium metal anode).

25 ENERGY STORAGE↗