Browsing by Author "Chen, CT"

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    Bulk and surface properties regulation of single/double perovskites to realize enhanced oxygen evolution reactivity
    (John Wiley & Sons, Inc, 2020-04-06) Sun, HS; Hu, B; Guan, DQ; Hu, ZW; Fei, LS; Li, MR; Peterson, VK; Lin, HJ; Chen, CT; Ran, R; Zhou, W; Shao, ZP
    Perovskite-based oxides have emerged as promising oxygen evolution reaction (OER) electrocatalysts. The performance is closely related to the lattice, electronic, and defect structure of the oxides, which determine surface and bulk properties and consequent catalytic activity and durability. Further, interfacial interactions between phases in a nanocomposite may affect bulk transportation and surface adsorption properties in a similar manner to phase doping except without solubility limits. Herein, we report the development of a single/double perovskite nanohybrid with limited surface self-reconstruction capability as an OER electrocatalyst. Such superior performance arises from a structure that maintains high crystallinity post OER catalysis, in addition to forming an amorphous layer following the self-reconstruction of a single perovskite structure during the OER process. In situ X-ray absorption near edge structure spectroscopy and high-resolution synchrotron-based X-ray diffraction reveal an amorphization process in the hybrid single/double perovskite oxide system that is limited in comparison to single perovskite amorphization, ensuring high catalytic activity. © 2020 Wiley-VCH Verlag GmbH & Co
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    Determination of hole distribution in Sr14-xCaxCu24O41 using soft x-ray absorption spectroscopy at the Cu L3 edge.
    (American Physical Society, 2013-07-22) Huang, MJ; Deng, G; Chin, YY; Hu, ZW; Cheng, JG; Chou, FC; Conder, K; Zhou, JS; Pi, TW; Goodenough, JB; Lin, HJ; Chen, CT
    The physical properties of Sr14-xCaxCu24O41 are determined by the hole distribution between the edge-shared CuO2 chain and the corner-shared Cu2O3 two-leg ladder, but inconsistent results on the hole distribution were obtained in various experimental works in recent decades. In this work we reinvestigate the hole distribution by soft x-ray absorption spectroscopy at the Cu L-3 edge. By comparing with the pure ladder and the pure chain systems, we can unambiguously distinguish between the hole distributions in the chain and the ladder. We have found that there are 5.3 holes in the edge-shared chain and 0.7 holes in the corner-shared ladder on average for Sr14Cu24O41. Upon Ca substitution, the holes gradually transfer from the edge-shared chain to the corner-shared ladder, and there are up to 1.21 holes in the corner-shared ladder for Sr1.8Ca12.2Cu24O41. © 2013, American Physical Society.
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    Direct evidence of Ni magnetic moment in TbNi2Mn—X-ray magnetic circular dichroism
    (Elsevier, 2014-12-01) Yu, DH; Huang, MJ; Su, HC; Lin, HJ; Chen, CT; Campbell, SJ; Wang, JL
    We have investigated the individual magnetic moments of Ni, Mn and Tb atoms in the intermetallic compound TbNi2Mn in the Laves phase (magnetic phase transition temperature TC ~131 K) by X-ray magnetic circular dichroism (XMCD) studies at 300 K, 80 K and 20 K. Analyses of the experimental results reveal that Ni atoms at 20 K in an applied magnetic field of 1 T carry an intrinsic magnetic moment of spin and orbital magnetic moment contributions 0.53±0.01 μB and 0.05±0.01 μB, respectively. These moment values are similar to those of the maximum saturated moment of Ni element. A very small magnetic moment of order <0.1 μB has been measured for Mn. This suggests that Mn is antiferromagnetically ordered across the two nearly equally occupied sites of 16d and 8a. A magnetic moment of up to ~0.3 μB has been observed for the Tb atoms. Identification of a magnetic moment on the Ni atoms has provided further evidence for the mechanism of enhancement of the magnetic phase transition temperature in TbNi2Mn compared with TbNi2 (TC~37.5 K) and TbMn2 (TC~54 K) due to rare earth–transition metal (R–T) and transition metal–transition metal (T–T) interactions. The behaviour of the X-ray magnetic circular dichroism spectra of TbNi2Mn at 300 K, 80 K and 20 K – above and below the magnetic ordering temperature TC ~131 K – is discussed. © 2014 Elsevier
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    High-performance perovskite composite electrocatalysts enabled by controllable interface engineering
    (John Wiley & Sons, Inc, 2021-06-17) Xu, XM; Pan, YL; Ge, L; Chen, YB; Mao, X; Guan, DQ; Li, MR; Zhong, YJ; Hu, ZW; Peterson, VK; Saunders, M; Chen, CT; Zhang, HJ; Ran, R; Du, AJ; Jiang, SP; Zhou, W; Shao, ZP
    Single-phase perovskite oxides that contain nonprecious metals have long been pursued as candidates for catalyzing the oxygen evolution reaction, but their catalytic activity cannot meet the requirements for practical electrochemical energy conversion technologies. Here a cation deficiency-promoted phase separation strategy to design perovskite-based composites with significantly enhanced water oxidation kinetics compared to single-phase counterparts is reported. These composites, self-assembled from perovskite precursors, comprise strongly interacting perovskite and related phases, whose structure, composition, and concentration can be accurately controlled by tailoring the stoichiometry of the precursors. The composite catalyst with optimized phase composition and concentration outperforms known perovskite oxide systems and state-of-the-art catalysts by 1–3 orders of magnitude. It is further demonstrated that the strong interfacial interaction of the composite catalysts plays a key role in promoting oxygen ionic transport to boost the lattice-oxygen participated water oxidation. These results suggest a simple and viable approach to developing high-performance, perovskite-based composite catalysts for electrochemical energy conversion. © 2021 Wiley-VCH GmbH
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    Unlocking fast and reversible sodium intercalation in NASICON Na4MnV(PO4)3 by fluorine substitution
    (Elsevier, 2021-11) Hou, J; Hadouchi, M; Sui, L; Liu, J; Tang, M; Kan, WH; Avdeev, M; Zhong, G; Liao, YK; Lai, YH; Chu, YH; Lin, HJ; Chen, CT; Hu, ZW; Huang, YH; Ma, J
    The exploitation of high energy and high power densities cathode materials for sodium ion batteries is a challenge. Na-super-ionic-conductor (NASICON) Na4MnV(PO4)3 is one of promising high-performance and low-cost cathode materials, however, still suffers from not reaching the theoretical capacity, low rate capability, and poor cycling stability. In this work, we deploy a novel sodium-deficient NASICON fluorinated phosphate cathode material for sodium ion batteries which demonstrates, notably, high energy and high power densities concomitant with high sodium diffusion kinetics. The enhanced performance of this novel Na3.85⬜0.15MnV(PO3.95F0.05)3 cathode was evidenced by demonstrating a relatively high energy density of ∼380 Wh kg−1 at low rate with much improved rate capability compared to non-doped Na4MnV(PO4)3, and long cycling life over 2000 cycles at high current rates. The structural investigation during battery operation using in situ x-ray diffraction (XRD) reveals bi-phase mechanism with high structural reversibility. The combined XRD and 23Na nuclear magnetic resonance (NMR) analyses demonstrate that the sodium extraction/insertion from Na2 is faster than Na1 site. These findings open promising prospects for unlocking of high energy and high power densities of NASICON phosphate materials by fluorine substitution towards high-performance sodium ion batteries. © 2021 Elsevier B.V.