Publications

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2020
Lee, W, Pan C-R, Nam H, Chou M-Y, Shih C-K.  2020.  Critical role of parallel momentum in quantum well state couplings in multi-stacked nanofilms: An angle resolved photoemission study, 2020. AIP AdvancesAIP Advances. 10(12):125211.: American Institute of Physics AbstractWebsite
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Chang, M-C, Ho P-H, Tseng M-F, Lin F-Y, Hou C-H, Lin I-K, Wang H, Huang P-P, Chiang C-H, Yang Y-C, Wang I-T, Du H-Y, Wen C-Y, Shyue J-J, Chen C-W, Chen K-H, Chiu P-W, Chen L-C.  2020.  Fast growth of large-grain and continuous MoS2 films through a self-capping vapor-liquid-solid method, 2020. 11(1):3682. AbstractWebsite

Most chemical vapor deposition methods for transition metal dichalcogenides use an extremely small amount of precursor to render large single-crystal flakes, which usually causes low coverage of the materials on the substrate. In this study, a self-capping vapor-liquid-solid reaction is proposed to fabricate large-grain, continuous MoS2 films. An intermediate liquid phase-Na2Mo2O7 is formed through a eutectic reaction of MoO3 and NaF, followed by being sulfurized into MoS2. The as-formed MoS2 seeds function as a capping layer that reduces the nucleation density and promotes lateral growth. By tuning the driving force of the reaction, large mono/bilayer (1.1 mm/200 μm) flakes or full-coverage films (with a record-high average grain size of 450 μm) can be grown on centimeter-scale substrates. The field-effect transistors fabricated from the full-coverage films show high mobility (33 and 49 cm2 V−1 s−1 for the mono and bilayer regions) and on/off ratio (1 ~ 5 × 108) across a 1.5 cm × 1.5 cm region.

Chang, H-C, Chen T-H, Sankar R, Yang Y-J, Chen L-C, Chen K-H.  2020.  Highly improved thermoelectric performance of BiCuTeO achieved by decreasing the oxygen content, 2020. 15:100248. AbstractWebsite

BiCuTeO is a promising thermoelectric material owing to its intrinsically low thermal conductivity and high carrier concentration. This study investigated the influence of stoichiometric oxygen deficiencies on the thermoelectric performance of BiCuTeO. Bulk BiCuTeO1−x (0.16 ≥ x) samples were prepared by a conventional solid state reaction and pelleted by hot pressing. Synchrotron X-ray diffraction, electron probe X-ray microanalysis, scanning electron microscopy, and transmission electron microscopy characterized the samples. A maximum value of 1.06 was achieved for the dimensionless figure of merit ZT at 673 K for BiCuTeO0.88, which is approximately 49% better than the current maximal ZT value for BiCuTeO. The power factor was noticeably improved owing to increases in the electrical conductivity and Seebeck coefficient. Moreover, the optimal oxygen deficiency could introduce nanoparticles, resulting in reduced thermal conductivity. The findings will be important for the future development of metal oxide thermoelectric materials for use in practical thermoelectric devices.

Shit, SC, Shown I, Paul R, Chen K-H, Mondal J, Chen L-C.  2020.  Integrated nano-architectured photocatalysts for photochemical CO2 reduction, 2020. Nanoscale. 12(46):23301-23332.: The Royal Society of Chemistry AbstractWebsite

Recent advances in nanotechnology, especially the development of integrated nanostructured materials, have offered unprecedented opportunities for photocatalytic CO2 reduction. Compared to bulk semiconductor photocatalysts, most of these nanostructured photocatalysts offer at least one advantage in areas such as photogenerated carrier kinetics, light absorption, and active surface area, supporting improved photochemical reaction efficiencies. In this review, we briefly cover the cutting-edge research activities in the area of integrated nanostructured catalysts for photochemical CO2 reduction, including aqueous and gas-phase reactions. Primarily explored are the basic principles of tailor-made nanostructured composite photocatalysts and how nanostructuring influences photochemical performance. Specifically, we summarize the recent developments related to integrated nanostructured materials for photocatalytic CO2 reduction, mainly in the following five categories: carbon-based nano-architectures, metal–organic frameworks, covalent-organic frameworks, conjugated porous polymers, and layered double hydroxide-based inorganic hybrids. Besides the technical aspects of nanostructure-enhanced catalytic performance in photochemical CO2 reduction, some future research trends and promising strategies are addressed.

Thang, NQ, Sabbah A, Chen L-C, Chen K-H, Hai LV, Thi CM, Viet PV.  2020.  Localized surface plasmonic resonance role of silver nanoparticles in the enhancement of long-chain hydrocarbons of the CO2 reduction over Ag-gC3N4/ZnO nanorods photocatalysts, 2020. :116049. AbstractWebsite

The conversion of CO2 into hydrocarbon fuels via the photocatalytic reaction route is considered a potential strategy to concurrently address serious energy crisis and greenhouse gas emission problems. Nevertheless, the generation of long-chain hydrocarbon products (Cn, n ≥ 2) from the visible-light-reactive photocatalytic CO2 reduction has also been considering a contemporary challenge. Herein, we indicate that Ag nanoparticles (Ag NPs) loaded gC3N4/ZnO nanorods heterojunction (Ag-gC3N4/ZnO NRs abbreviation) has extended photoactive range and enhanced specific surface area. The combination of Ag NPs and gC3N4/ZnO NRs significantly enhances photocatalytic CO2 reduction efficiency to form the acetone product. Detail, the acetone production efficiency of Ag-gC3N4/ZnO NRs is 8.4 and 7.5 times higher than pure ZnO NRs and gC3N4/ZnO NRs at the same condition, respectively. This study represents a potential approach toward higher-energy-value hydrocarbons production and greenhouse gas emission mitigation.

Billo, T, Shown I, kumar Anbalagan A, Effendi TA, Sabbah A, Fu F-Y, Chu C-M, Woon W-Y, Chen R-S, Lee C-H, Chen K-H, Chen L-C.  2020.  A mechanistic study of molecular CO2 interaction and adsorption on carbon implanted SnS2 thin film for photocatalytic CO2 reduction activity, 2020. 72:104717. AbstractWebsite

Gas-phase photocatalytic reactions to convert carbon dioxide and water into oxygen and hydrocarbons are the foundation of life on earth. However, the efficiency of photosynthesis is relatively low (~1%), which leaves much room for artificial photosynthesis to reach the benchmark of the solar cells (>15%). In this work, carbon implanted SnS2 thin films (C–SnS2) were prepared to study photocatalytic activity and adsorbate-catalyst surface interactions during CO2 photoreduction. The electron density distribution in C–SnS2 and its contribution toward the photogenerated charge transfer process has been analyzed by the angle-dependent X-ray absorption near-edge structure (XANES) study. The C–SnS2 surface affinity toward the CO2 molecule was monitored by in-situ dark current and Raman spectroscopy measurements. By optimizing the dose during ion implantation, SnS2 thin film with 1 wt% carbon incorporation shows 108 times enhancement in the CO2 conversion efficiency and more than 89% product selectivity toward CH4 formation compared with the as-grown SnS2 without carbon incorporation. The improved photocatalytic activity can be ascribed to enhanced light harvesting, pronounced charge-transfer between SnS2 and carbon with improved carrier separation and the availability of highly active carbon sites that serve as favorable CO2 adsorption sites.

Howlader, S, Vasudevan R, Jarwal B, Gupta S, Chen K-H, Sachdev K, Banerjee MK.  2020.  Microstructure and mechanical stability of Bi doped Mg2Si0.4Sn0.6 thermoelectric material, 2020. 818:152888. AbstractWebsite

Bi doped Mg2Si0.4Sn0.6 had been synthesised in a high energy ball mill followed by compaction using a sintering hot press. The structural and compositional characterization of sintered mass indicated the formation of a highly densified single-phase product. The microstructure of the hot-pressed samples had been critically assessed. Thermoelectric properties were measured between room temperature and 723 K. A decrease in electrical conductivity was found with the increase in temperature but the Seebeck coefficient showed a reverse trend justifying the attainment of degenerate semiconducting behaviour. Meanwhile, the lattice thermal conductivity was subdued to 1.5 W/mK at 623 K. However, the highest zT value of 0.8 was achieved at 723 K. Moreover, the detailed X-ray photoelectron spectroscopic analysis was carried for the determination of binding energy of the constituent elements in the experimental alloy; it also provided the correct estimation of atomic percentage of the concerned elements. The Raman spectrum revealed a shift in F2g peak with respect to that of Mg2Sn and Mg2Si in correspondence with the composition of the synthesised alloy. The synthesised alloy showed micro and nano hardness of 3.7 and 4.03 GPa respectively, which implies that good mechanical strength could be achieved in the synthesised alloy.

Huang, W-F, Chang S-T, Huang H-C, Wang C-H, Chen L-C, Chen K-H, Lin MC.  2020.  On the Reduction of O2 on Cathode Surfaces of Co–Corrin and Co–Porphyrin: A Computational and Experimental Study on Their Relative Efficiencies in H2O/H2O2 Formation, 2020. The Journal of Physical Chemistry CThe Journal of Physical Chemistry C. 124(8):4652-4659.: American Chemical Society AbstractWebsite
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Lien, H-T, Chang S-T, Chen P-T, Wong DP, Chang Y-C, Lu Y-R, Dong C-L, Wang C-H, Chen K-H, Chen L-C.  2020.  Probing the active site in single-atom oxygen reduction catalysts via operando X-ray and electrochemical spectroscopy, 2020. 11(1):4233. AbstractWebsite

Nonnoble metal catalysts are low-cost alternatives to Pt for the oxygen reduction reactions (ORRs), which have been studied for various applications in electrocatalytic systems. Among them, transition metal complexes, characterized by a redox-active single-metal-atom with biomimetic ligands, such as pyrolyzed cobalt–nitrogen–carbon (Co–Nx/C), have attracted considerable attention. Therefore, we reported the ORR mechanism of pyrolyzed Vitamin B12 using operando X-ray absorption spectroscopy coupled with electrochemical impedance spectroscopy, which enables operando monitoring of the oxygen binding site on the metal center. Our results revealed the preferential adsorption of oxygen at the Co2+ center, with end-on coordination forming a Co2+-oxo species. Furthermore, the charge transfer mechanism between the catalyst and reactant enables further Co–O species formation. These experimental findings, corroborated with first-principle calculations, provide insight into metal active-site geometry and structural evolution during ORR, which could be used for developing material design strategies for high-performance electrocatalysts for fuel cell applications.

Bayikadi, KS, Wu CT, Chen L-C, Chen K-H, Chou F-C, Sankar R.  2020.  Synergistic optimization of thermoelectric performance of Sb doped GeTe with a strained domain and domain boundaries, 2020. Journal of Materials Chemistry A. 8(10):5332-5341.: The Royal Society of Chemistry AbstractWebsite

In addition to the Ge-vacancy control of GeTe, the antimony (Sb) substitution of GeTe for the improvement of thermoelectric performance is explored for Ge1−xSbxTe with x = 0.08–0.12. The concomitant carrier concentration (n) and the aliovalent Sb ion substitution led to an optimal doping level of x = 0.10 to show ZT ∼ 2.35 near ∼800 K, which is significantly higher than those single- and multi-element substitution studies of the GeTe system reported in the literature. In addition, Ge0.9Sb0.1Te demonstrates an impressively high power factor of ∼36 μW cm−1 K−2 and a low thermal conductivity of ∼1.1 W m−1 K−1 at 800 K. The enhanced ZT level for Ge0.9Sb0.1Te is explained through a systematic investigation of micro-structural change and strain analysis from room temperature to 800 K. A significant reduction of lattice thermal conductivity (κlat) is identified and explained by the Sb substitution-introduced strained and widened domain boundaries for the herringbone domain structure of Ge0.9Sb0.1Te. The Sb substitution created multiple forms of strain near the defect centre, the herringbone domain structure, and widened tensile/compressive domain boundaries to support phonon scattering that covers a wide frequency range of the phonon spectrum to reduce lattice thermal conductivity effectively.

Wei, Y-C, Hsiao Y-F, Wu B-H, Tsai P-J, Chen Y-C.  2020.  Broadband coherent optical memory based on electromagnetically induced transparency. Phys. Rev. A. 102, 063720Link
Lee, T.-Y., JTLCVSTPK.  2020.  Carbon dot nanoparticles exert inhibitory effects on human platelets and reduce mortality in mice with acute pulmonary thromboembolism. AbstractWebsite

The inhibition of platelet activation is considered a potential therapeutic strategy for the treatment of arterial thrombotic diseases; therefore, maintaining platelets in their inactive state has garnered much attention. In recent years, nanoparticles have emerged as important players in modern medicine, but potential interactions between them and platelets remain to be extensively investigated. Herein, we synthesized a new type of carbon dot (CDOT) nanoparticle and investigated its potential as a new antiplatelet agent. This nanoparticle exerted a potent inhibitory effect in collagen-stimulated human platelet aggregation. Further, it did not induce cytotoxic effects, as evidenced in a lactate dehydrogenase assay, and inhibited collagen-activated protein kinase C (PKC) activation and Akt (protein kinase B), c-Jun N-terminal kinase (JNK), and p38 mitogen-activated protein kinase (MAPK) phosphorylation. The bleeding time, a major side-effect of using antiplatelet agents, was unaffected in CDOT-treated mice. Moreover, our CDOT could reduce mortality in mice with ADP-induced acute pulmonary thromboembolism. Overall, CDOT is effective against platelet activation in vitro via reduction of the phospholipase C/PKC cascade, consequently suppressing the activation of MAPK. Accordingly, this study affords the validation that CDOT has the potential to serve as a therapeutic agent for the treatment of arterial thromboembolic disorders. © 2020 by the authors.

Wang, S, Scholes GD *, Hsu L-Y*.  2020.  Coherent-to-Incoherent Transition of Molecular Fluorescence Controlled by Surface Plasmon Polaritons. J. Phys. Chem. Lett.. 11:5948-5955. AbstractWebsite

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Tsai, Y‐F, Wei P‐C, Chang L, Wang K‐K, Yang C‐C, Lai Y‐C, Hsing C‐R, Wei C‐M, He J, Snyder JG, Wu H‐J.  2020.  Compositional Fluctuations Locked by Athermal Transformation Yielding High Thermoelectric Performance in GeTe. Advanced Materials.
Veerakumar, P., DLNK-C.  2020.  Computational and experimental analysis of carbon functional nanomaterials. Abstract

Density functional theory (DFT) as one of molecular simulation techniques has been widely used to become rapidly a powerful tool for research and technology development for the past three decades. In particular, the DFT-based theoretical and fundamental knowledge have shed light on our understanding of the fundamental surface science, catalysis, sensors, materials science, and biology. Oxygen, nitrogen, boron, phosphorus, and sulfur are the most common heteroatoms introduced on the functional carbon nanomaterials surface with different surface functionalities. This book chapter aims to provide a pedagogical narrative of the DFT and relevant computational methods applied for surface chemistry, homogeneous/heterogeneous catalysis, and the fluorescence-based sensing properties of carbon nanomaterials. We overview several representative case studies associated with energy and chemicals production and discuss relevant principles of computationally driven carbon nanomaterials design.

Lee, H-W, Hsing C-R, Chang C-M, Wei C-M.  2020.  Electronic structures of 24-valence-electron full Heusler compounds investigated by density functional and GW calculations. Journal of Physics: Condensed Matter. 32:175501. Abstract

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Veerakumar, P., SCPLAS-M.  2020.  Fabrication of Platinum-Rhenium Nanoparticle-Decorated Porous Carbons: Voltammetric Sensing of Furazolidone. AbstractWebsite

This study discusses the prospect of using biomass waste material, such as Cassia fistula (golden shower) fruit, as a carbon precursor in the development of new carbon material for the sustainable electrochemical sensor application. We successfully synthesized platinum-rhenium nanoparticles decorated on a porous activated carbon (Pt-Re NP/PAC) nanocomposite through the incorporation of metal precursors such as platinum(II) acetylacetonate (Pt(acac)2) and dirhenium decacarbonyl (Re2(CO)10) via a facile thermal reduction process. A variety of physicochemical and electrochemical methods were employed to characterize the morphology, structural, and electrochemical properties of the Pt-Re NP/PAC material. We then looked into the analytical behavior and applications of GCE modified with Pt-Re NP/PAC (Pt-Re NP/PAC/GCE) for the determination of furazolidone (chemotherapy drug) by employing different voltammetric techniques. The influence of experimental conditions such as scan rate, pH, accumulation time, amount of the modifier, and sample concentration on the peak current of the furazolidone was studied. The proposed drug sensor exhibited a wide linear range (WLR) for furazolidone in 0.05 M phosphate-buffered saline (PBS, pH 7.0) from 1.0 to 299 μM with a limit of detection (LOD) of 75.5 nM and appreciable sensitivity (5.52 μA μM-1 cm-2) which were calculated from linear sweep voltammetry (LSV). In addition, these analytical parameters including WLR, sensitivity, and LOD were estimated to be 0.2-117.7 μM, 19.20 μA μM-1 cm-2, and 20.8 nM and were obtained using differential pulse voltammetry (DPV). Therefore, the prepared Pt-Re NP/PAC modified sensor could be a potential candidate for the determination of furazolidone in pharmaceutical formulation, human urine, and blood serum samples, and the results are appreciable. Copyright © 2020 American Chemical Society.

Lin, H-Y, Song BF, Ni* C-K.  2020.  Fluorescence quantum yields of matrices used in ultravioletmatrix-assisted laser desorption/ionization.. Rapid Commun Mass Spectrom.. 34:e8846.
Hsu, L-Y*, Yen H-C, Lee M-W, Sheu Y-lin, Chen P-C, Dai H*, Chen C-C*.  2020.  Large-Scale Inhomogeneous Fluorescence Plasmonic Silver Chips: Origin and Mechanism. Chem. 6:1-13. AbstractWebsite

Summary Large-scale inhomogeneous plasmonic metal chips have been demonstrated as a promising platform for biochemical sensing, but the origin of their strong fluorescence enhancements and average gap dependence is a challenging issue due to the complexity of modeling tremendous molecules within inhomogeneous gaps. To address this issue, we bridged microscopic mechanisms and macroscopic observations, developed a kinetic model, and experimentally investigated the fluorescence enhancement factors of IR800-streptavidin immobilized on metal nanoisland films (NIFs). Inspired by the kinetic model, we controlled the distribution of IR800-streptavidin within the valleys of NIFs by regioselective modification and achieved the fluorescence intensity enhancement up to 488-fold. The kinetic model allows us to qualitatively explain the mechanism of fluorescence intensity enhancements and quantitatively predict the trend of experimental enhancement factors, thereby determining the design principles of the plasmonic metal chips. Our study provides one key step further toward the sensing applications of large-scale plasmonic metal chips.

Wei, Y-C, Lin S-X, Tsai P-J, Chen Y-C.  2020.  Memory-based optical polarization conversion in a double-Λ atomic system with degenerate Zeeman states. Sci Rep. 10, 13990 (2020) Link
C.R.P.Inbaraj, Mathew RJ, Kumar UR, Sankar R, Kataria M, Lin HY, Cheng H-Y, Lin K-H, Lin H-I, Liao Y-M, Chou FC, Chen Y-T, Lee C-H, Chen Y-F.  2020.  Modulating Charge Separation with Hexagonal Boron Nitride Mediation in Vertical Van der Waals Heterostructures. ACS Appl. Mater. Interfaces . 12:26213−26221.view
Chuang, Y-T, Chen S-D, Huang W-C, Shen T-L, Chang M-S, Chen Y-F, Hsieh Y-P, Chang Y-H, Hofmann M.  2020.  Multilevel Optical Labeling by Spectral Luminescence Control in Nanodiamond Color Centers. ACS Applied Materials & Interfaces. 12(43):49006-49011.
Y.-C.Chang, Tseng C-A, Lee C-P, Ann S-B, Huang Y-J, Ho KC, Chen Y-T.  2020.  N- and S-codoped graphene hollow nanoballs as an efficient Pt-free electrocatalyst for dye-sensitized solar cells. J.Pow. Sour.. :227470.view