Engineering topics

Liu, Xiaosong

Publications and source records attributed to Liu, Xiaosong.

4 records

DOE OSTI2024

Quantitative Identification of Dopant Occupation in Li‐Rich Cathodes

Elemental doping is widely used to improve the performance of cathode materials in lithium‐ion batteries. However, macroscopic/statistical investigation on how doping sites are distributed in the material lattice, despite being a key prerequisite for understanding and manipulating the doping effect, has not been effectively established. Herein, to solve this predicament, a universal strategy is proposed to quantitatively identify the locations of Al and Mg dopants in lithium‐rich layered oxides (LLOs). Solid evidence confirms that Al prefers to occupy the transition metal (TM) layer, while Mg evenly occupies both TM and Li layers. As a result, Mg significantly reduces the thickness of LiO 2 slabs at room temperature, which will increase the energy barrier of oxygen activation and enhance the structure stability of LLOs. The suppressed oxygen activity in Mg‐doped LLO can be kinetically unlocked at 55 °C. The different characteristics of Al and Mg enlighten an Al/Mg co‐doping strategy to optimize LLOs, which significantly improves the cycle performance while lifting the capacity. In conclusion, these insights from the quantitative identification of doping sites shed light on the manipulation of doping effects toward better cathodes.

25 ENERGY STORAGE↗

DOE OSTI2024

Flexible Soft X-Ray Image Sensors based on Metal Halide Perovskites With High Quantum Efficiency

Soft X-ray imaging is a powerful tool to explore the structure of cells, probe material with nanometer resolution, and investigate the energetic phenomena in the universe. Conventional soft X-ray image sensors are by and large Si-based charge coupled devices that suffer from low frame rates, complex fabrication processes, mechanical inflexibility, and required cooling below -60 °C. Here, a soft X-ray photodiode is reported based on low-cost metal halide perovskite with comparable performance to commercial Si-based device. Nanothrough network electrode minimized the optical loss due to the shadowing of insensitive layers, while a multidimensional perovskite heterojunction is generated to reduce the photo-generated carrier loss. Further, this strategy promoted a record quantum efficiency of 8 × 10 3 % without cooling, several orders of magnitude greater than the previously achieved. Flexible and curved soft X-ray imaging arrays are fabricated based on this high-performance device structure, demonstrating stable soft X-ray response and sharp imaging capabilities. This work highlights the low-cost and efficient perovskite photodiode as a strong candidate for the next-generation soft X-ray image sensors.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Enhanced orbital anisotropy through the proximity to a SrTiO 3 layer in the perovskite iridate superlattices

We have used angle-dependent soft x-ray absorption spectroscopy (XAS) at the O K edge and first-principles calculations to investigate the electronic structures of iridate-based superlattices ( SrIr O 3 ) m / ( SrTi O 3 ) ( m = 1 , 2, 3, and ∞). We focus on the pre-edge Ir 5 d t 2 g – O 2 p orbital hybridization feature in the XAS spectra. By varying the measurement geometry relative to the incident photon polarization, we are able to extract the dichroic contrast and observe the systematic increase in the anisotropy of Ir 5 d orbitals as m decreases. First-principles calculations elucidate the orbital anisotropy coming mainly from the enhanced out-of-plane compression of Ir O 6 octahedra in the SrIr O 3 layers that are adjacent to the inserted SrTi O 3 layers. As m decreases, the increased volume fraction of these interfacial SrIr O 3 layers and their contact with the SrTi O 3 layers within the ( SrIr O 3 ) m / ( SrTi O 3 ) supercell lead to enhanced orbital anisotropy. Furthermore, the tilt and rotation of Ir O 6 octahedra are shown to be essential to understand the subtle orbital anisotropy in these superlattices, and constraining these degrees of freedom will give an incorrect trend. Overall, our results demonstrate that the structural constraint from the inserted SrTi O 3 layers, in addition to other electronic means such as polar interface and charge transfer, can serve as a knob to control the orbital degree of freedom in these iridate-based superlattices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Deciphering the Solvent Effect for the Solvation Structure of Ca 2+ in Polar Molecular Liquids

Although the crystal structures for many inorganic compounds are readily available, researchers are still working hard to understand the relations between the structures and chemical properties of solutions because most of the chemical reactions take place in solutions. A huge amount of effort has been put toward modeling the ion solvation structure from the perspectives of both experiments and theories. In this study, the solvation structures of Ca 2+ ions in aqueous and alcoholic solutions at different concentrations were carefully evaluated by Ca K-edge X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) analyses. Further, density functional theory (DFT) calculations were also performed to correlate the results with the experimental data and then further extended to other similar systems. It was found that the number of coordinating solvent molecules decreases with increasing Ca 2+ concentration and increasing solvent molecule sizes. From the EXAFS data, it was observed that the first solvation shell of Ca 2+ splits into two Ca-O distances in a methanol solution and the counter ion Cl - might also be within the first shell at high concentrations. For the first time, the effects of solvents with different polarities and sizes on the ion solvation environment were systematically evaluated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗