Browsing by Author "Zheng, Yongping"
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Item Kinetic Stability of Bulk LiNiO₂ and Surface Degradation by Oxygen Evolution in LiNiO₂-Based Cathode Materials(Wiley-VCH Verlag Gmbh, 2018-11-02) Kong, Fantai; Liang, Chaoping; Wang, Luhua; Zheng, Yongping; Perananthan, Sahila; Longo, Roberto C.; Ferraris, John P.; Kim, Moon J.; Cho, Kyeongjae; Kong, Fantai; Liang, Chaoping; Wang, Luhua; Zheng, Yongping; Perananthan, Sahila; Longo, Roberto C.; Ferraris, John P.; Kim, Moon J.; Cho, KyeongjaeCapacity degradation by phase changes and oxygen evolution has been the largest obstacle for the ultimate commercialization of high-capacity LiNiO₂-based cathode materials. The ultimate thermodynamic and kinetic reasons of these limitations are not yet systematically studied, and the fundamental mechanisms are still poorly understood. In this work, both phenomena are studied by density functional theory simulations and validation experiments. It is found that during delithiation of LiNiO₂, decreased oxygen reduction induces a strong thermodynamic driving force for oxygen evolution in bulk. However, oxygen evolution is kinetically prohibited in the bulk phase due to a large oxygen migration kinetic barrier (2.4 eV). In contrast, surface regions provide a larger space for oxygen migration leading to facile oxygen evolution. These theoretical results are validated by experimental studies, and the kinetic stability of bulk LiNiO₂ is clearly confirmed. Based on these findings, a rational design strategy for protective surface coating is proposed.Item Quantum Transport and Band Structure Evolution under High Magnetic Field in Few-Layer Tellurene(American Chemical Society) Qiu, G.; Wang, Y.; Nie, Yifan; Zheng, Yongping; Cho, Kyeongjae; Wu, W.; Ye, P. D.; 0000-0003-4771-3633 (Nie, Y); 0000-0003-2698-7774 (Cho, K); 369148996084659752200 (Cho, K); Nie, Yifan; Zheng, Yongping; Cho, KyeongjaeQuantum Hall effect (QHE) is a macroscopic manifestation of quantized states that only occurs in confined two-dimensional electron gas (2DEG) systems. Experimentally, QHE is hosted in high-mobility 2DEG with large external magnetic field at low temperature. Two-dimensional van der Waals materials, such as graphene and black phosphorus, are considered interesting material systems to study quantum transport because they could unveil unique host material properties due to the easy accessibility of monolayer or few-layer thin films at the 2D quantum limit. For the first time, we report direct observation of QHE in a novel low-dimensional material system, tellurene. High-quality 2D tellurene thin films were acquired from recently reported hydrothermal method with high hole mobility of nearly 3000 cm2/(V s) at low temperatures, which allows the observation of well-developed Shubnikov-de Haas (SdH) oscillations and QHE. A four-fold degeneracy of Landau levels in SdH oscillations and QHE was revealed. Quantum oscillations were investigated under different gate biases, tilted magnetic fields, and various temperatures, and the results manifest the inherent information on the electronic structure of Te. Anomalies in both temperature-dependent oscillation amplitudes and transport characteristics were observed that are ascribed to the interplay between the Zeeman effect and spin-orbit coupling, as depicted by the density functional theory calculations. ©2018 American Chemical Society.Item Superior Low-Temperature NO Catalytic Performance of PrMn₂O₅ over SmMn₂O₅ Mullite-Type Catalysts(Royal Society of Chemistry, 2019) Thampy, Sampreetha; Ashburn, Nickolas; Liu, C.; Xiong, K.; Dillon, Sean; Zheng, Yongping; Chabal, Yves J.; Cho, Kyeongjae; Hsu, Julia W. P.; 0000-0002-7821-3001 (Hsu, JWP); 0000-0002-6435-0347 (Chabal, YJ); 0000-0003-2698-7774 (Cho, K); 369148996084659752200 (Cho, K); Thampy, Sampreetha; Ashburn, Nickolas; Dillon, Sean; Zheng, Yongping; Chabal, Yves J.; Cho, Kyeongjae; Hsu, Julia W. P.By studying their surface chemistry, metal-oxygen bond strength, and critical energy barrier heights, we elucidate the differences in the NO oxidation catalytic performance of PrMn₂O₅ and SmMn₂O₅ mullite-type oxides. The 50% conversion temperature is lower (230 °C vs. 275 °C) and the maximum conversion efficiency is higher (81% at 282 °C vs. 68% at 314 °C) for PrMn₂O₅ compared to SmMn₂O₅, despite having a ∼15% lower specific surface area. Furthermore, PrMn₂O₅ exhibits higher maximum efficiency compared to Pt/Al₂O₃. Combined experimental and theoretical findings indicate that the superior catalytic performance of PrMn₂O₅ at low temperatures arises from the presence of more labile and reactive surface lattice oxygen due to weaker Mn-O bond strength and lower thermal stability of surface NOₓ ad-species. ©2019 The Royal Society of Chemistry.Item Theoretical and Experimental Study of Catalysis on Clean Energy Applications(2018-12) Zheng, Yongping; Cho, KyeongjaeCatalysis is of pivotal importance to many aspects of modern society, from chemicals synthesis to energy production and to pollutants remediation. Along with the growing world population and industrialization scale, rapid increases in global energy demands and environmental issues create a formidable challenge in designing new catalysts, which should be more active, more selective, more stable, and preferably comprised of earth-abundant elements. Traditional trialand-error methods no longer meet this fast increasing requirement, which typically takes a long period for the basic research in materials design translating to manufacturing. Computational modeling can accelerate this process and greatly shorten the timescale. In this dissertation, I will introduce our recent achievements in catalyst development for oxygen reduction reaction (ORR) in fuel cell and Li-air battery, and oxidation reaction in diesel exhaust by integrating theory and experiment. The density functional theory (DFT) method is used to describe surface chemical reactions in atomic scale and to uncover the underlying principles that govern the catalytic activity. We further validate the theoretical predictions through experimental results, and develop general descriptors for new catalysts design and optimization.