| 1. |
- Chen, Zhiwen, et al.
(författare)
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Interface engineering of NiS@MoS2 core-shell microspheres as an efficient catalyst for hydrogen evolution reaction in both acidic and alkaline medium
- 2021
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Ingår i: Journal of Alloys and Compounds. - : ELSEVIER SCIENCE SA. - 0925-8388 .- 1873-4669. ; 853
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Tidskriftsartikel (refereegranskat)abstract
- Electrochemical splitting of water is one of the most reliable and effective ways for the sustainable production of pure hydrogen on a large scale, while the core of this technology lies in the development of highly active non-noble-metal-based electrocatalysts to lower the large dynamic overpotentials of electrode materials. Here, an interface engineering strategy is demonstrated to construct an efficient and stable catalyst based on NiS@MoS2 core-shell hierarchical microspheres for the hydrogen evolution reactions (HER). The ultrathin MoS2 nanosheets in-situ grow on the surface of NiS hierarchical micro-sized spheres constructed by porous nanoplates, endowing the composites with rich interfaces, well-exposed electroactive edges, high structural porosity and fast transport channels. These advantages are favorable for the improvement of catalytic sites and the transport of catalysis-relevant species. More importantly, the intimate contact between MoS2 nanosheets and NiS nanoplates synergistically favors the chemical sorption of hydrogen intermediates, thereby reducing the reaction barrier and accelerating the HER catalytic process. As a result, the optimized NiS@MoS2 catalyst manifests impressive HER activity and durability, with a low overpotential of 208 mV in 0.5 M H2SO4 and 146 mV in 1.0 M KOH at 10 mA cm(-2), respectively. This work not only provides an effective way to construct core-shell hierarchical microspheres but also a multiscale strategy to regulate the electronic structure of heterostructured materials for energy-related applications. (C) 2020 Elsevier B.V. All rights reserved.
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| 2. |
- Chen, Zhiwen, et al.
(författare)
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Well-defined CoSe2@MoSe2 hollow heterostructured nanocubes with enhanced dissociation kinetics for overall water splitting
- 2020
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Ingår i: Nanoscale. - : ROYAL SOC CHEMISTRY. - 2040-3364 .- 2040-3372. ; 12:1, s. 326-335
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Tidskriftsartikel (refereegranskat)abstract
- Hollow heterostructures have tremendous advantages in electrochemical energy storage and conversion areas due to their unique structure and composition characteristics. Here, we report the controlled synthesis of hollow CoSe2 nanocubes decorated with ultrathin MoSe2 nanosheets (CoSe2@MoSe2) as an efficient and robust bifunctional electrocatalyst for overall water splitting in a wide pH range. It is found that integrating ultrathin MoS2 nanosheets with hollow CoSe2 nanocubes can provide abundant active sites, promote electron/mass transfer and bubble release and facilitate the migration of charge carriers. Additionally, the surface electron coupling in the heterostructures enables it to serve as a source of sites for H+ and/or OH- adsorption, thus reducing the activation barrier for water molecules adsorption and dissociation. As a result, the title compound, CoSe2@MoSe2 hollow heterostructures, exhibits an overpotential of 183 mV and 309 mV at a current density of 10 mA cm(-2) toward hydrogen evolution reactions and oxygen evolution reactions in 1.0 M KOH, respectively. When applied as both cathode and anode for overall water splitting, a low battery voltage of 1.524 V is achieved along with excellent stability for at least 12 h. This work provides a new idea for the design and synthesis of high-performance catalysts for electrochemical energy storage and conversion.
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| 3. |
- Cheng, Chunyan, et al.
(författare)
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Near-Unity Quantum Yield ZnSeTe Quantum Dots Enabled by Controlling Shell Growth for Efficient Deep-Blue Light-Emitting Diodes
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Ingår i: Advanced Functional Materials. - 1616-301X.
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Tidskriftsartikel (refereegranskat)abstract
- Core–shell structural ZnSeTe/ZnSe/ZnS quantum dots (QDs) have attracted great attention for advanced illumination and displays because of their environmentally friendly composition, but still suffering from poor photoluminescence (PL) and electroluminescence (EL) performance due to severe non-radiative charge recombination. Herein, a stepwise injection shell growth process to manipulate the monomer concentration and ensure adequate growth interval is devised, which enables the controllable uniform epitaxial growth of ZnSe and ZnS shells on the ZnSeTe core, thus relieving the lattice distortion and defects to greatly suppress the non-radiative charge recombination. The ZnSeTe/ZnSe/ZnS QDs presented deep-blue emission at 448 nm with narrow full width at half maximum (FWHM, 23 nm), and near-unity PL quantum yield (PLQY, ≈100%) The light-emitting diodes (LEDs) based on the QDs exhibited a high external quantum efficiency (EQE) of 10.9%, a maximum brightness of 10240 cd cm−2, and a high current efficiency of 7.9 cd A−1, demonstrating a good performance for deep blue QDs LEDs (QLEDs) This shell growth strategy will be an effective approach to achieving efficient QDs and QLEDs.
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| 4. |
- Gao, Yan, et al.
(författare)
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Differential accumulation and elimination behavior of perfluoroalkyl acid isomers in occupational workers in a manufactory in China
- 2015
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 49:11, s. 6953-6962
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Tidskriftsartikel (refereegranskat)abstract
- In this study, serum and urine samples were collected from 36 occupational workers in a fluorochemical manufacturing plant in China from 2008 to 2012 to evaluate the body burden and possible elimination of linear and branched perfluoroalkyl acids (PFAAs). Indoor dust, total suspended particles (TSP), diet, and drinking water samples were also collected to trace the occupational exposure pathway to PFAA isomers. The geometric mean concentrations of perfluorooctanesulfonate (PFOS), perfluorooctanoate (PFOA), and perfluorohexanesulfonate (PFHxS) isomers in the serum were 1386, 371, and 863 ng mL(-1), respectively. The linear isomer of PFOS, PFOA, and PFHxS was the most predominant PFAA in the serum, with mean proportions of 63.3, 91.1, and 92.7% respectively, which were higher than the proportions in urine. The most important exposure routes to PFAA isomers in the occupational workers were considered to be the intake of indoor dust and TSP. A renal clearance estimation indicated that branched PFAA isomers had a higher renal clearance rate than did the corresponding linear isomers. Molecular docking modeling implied that linear PFOS (n-PFOS) had a stronger interaction with human serum albumin (HSA) than branched isomers did, which could decrease the proportion of n-PFOS in the blood of humans via the transport of HSA.
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| 5. |
- Huang, Shoushuang, et al.
(författare)
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An advanced electrocatalyst for efficient synthesis of ammonia based on chemically coupled NiS@MoS2 heterostructured nanospheres
- 2021
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Ingår i: Sustainable Energy & Fuels. - : Royal Society of Chemistry. - 2398-4902. ; 5:10, s. 2640-2648
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Tidskriftsartikel (refereegranskat)abstract
- The electrochemical reduction of nitrogen, as a sustainable alternative to the known Haber-Bosch process, possesses promising application prospects in the development of renewable energy storage systems. However, the yield of NH3 and Faraday efficiency are usually very low owing to the loss of active electrocatalysts and competitive hydrogen evolution reactions. Herein, uniform NiS@MoS2 core-shell microspheres are controllably prepared as a potential catalyst for an ambient electrocatalytic N-2 reduction reaction. The NiS@MoS2 microspheres possess highly active intrinsic, sufficient accessible active sites, high structural porosity, and convenient transport channels, consequently boosting the transmission of electrons and mass. Additionally, the interfacial interaction between NiS and MoS2 facilitates electron transfer, which further improves the catalytic activity by optimizing the free energies of reaction intermediates. As a result, the titled NiS@MoS2 shows excellent electrochemical activity and selectivity, capable of achieving a relatively high NH3 yield of 9.66 mu g h(-1) mg(cat)(-1) at -0.3 V (vs. the reversible hydrogen electrode, RHE) and a high FE of 14.8% at -0.1 V vs. RHE in 0.1 M Na2SO4. The work demonstrated here may open a new avenue for the rational design and synthesis of catalysts for the electrochemical synthesis of ammonia.
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| 6. |
- Huang, Shoushuang, et al.
(författare)
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Enhancing electroreduction activity and selectivity of N2-to-NH3 through proton-feeding adjustments in Ag@AgP2@Ni-CoP@C core-shell nanowires
- 2023
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Ingår i: Applied Catalysis B. - : ELSEVIER. - 0926-3373 .- 1873-3883. ; 337
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Tidskriftsartikel (refereegranskat)abstract
- The synthesis of NH3 via electrochemical N2 fixation at ambient conditions has been proposed as a promising alternative to the traditional Haber-Bosch process. However, the development of highly efficient and selective electrocatalysts remains a challenge. In this study, uniform Ag@AgP2 @Ni-CoP@C core-shell nanowires were synthesized using a template-engaged strategy. The merging of conductive Ag core with active AgP2 and porous carbon-coated Ni-doped CoP shells favors the mass and electron transfers, effectively lowering the activation energy toward the reduction of N2 to NH3. Density functional theory (DFT) calculations further indicates that the sandwiched AgP2 layer plays crucial roles in promoting electrocatalytic kinetics and suppressing the competitive hydrogen evolution reactions. Benefiting from these advantages, the titled catalyst achieved a high NH3 yield of 16.84 & mu;g h-1 mg-1 cat. at-0.4 V (vs. reversible hydrogen electrode, RHE) and a high Faradaic efficiency of 21.7 % at-0.3 V vs. RHE, as well as high electrochemical and structure stability.
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| 7. |
- Huang, Shoushuang, et al.
(författare)
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Synergistically modulating electronic structure of NiS2 hierarchical architectures by phosphorus doping and sulfur-vacancies defect engineering enables efficient electrocatalytic water splitting
- 2021
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Ingår i: Chemical Engineering Journal. - : ELSEVIER SCIENCE SA. - 1385-8947 .- 1873-3212. ; 420
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Tidskriftsartikel (refereegranskat)abstract
- The synergistic achievement of heteroatom doping, defect engineering and appropriate structural design is efficient to adjust and boost the catalytic performance of catalysts yet challenging. Herein, phosphorus (P)-doped NiS2 hierarchical architectures with sulfur vacancies are synthesized via a Prussian-blue-analogue-sacrificed strategy followed by a phosphidation process. By modulation of P doping and sulfur vacancies, the optimal catalyst manifests outstanding electrocatalytic activities, affording low overpotentials of 73 mV at 10 mA cm-2 for hydrogen evolution reaction (HER), and 255 mV at 20 mA cm-2 for oxygen evolution reaction (OER), respectively. Density functional theory calculations certify that the P dopant not only serves as the new active sites, but also activates the electrochemical activity of neighboring Ni and S sites. Moreover, the synergistic effect of P-doping and sulfur vacancies further improve electrochemical activities of HER and OER by optimizing the adsorption free energy of hydrogen (Delta GH*) and oxygen-containing intermediates (OH*, O* and OOH*), respectively. This finding provides a directive strategy to achieve efficient non-noble metal catalysts for energy conversion and storage.
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| 8. |
- Jia, Min, et al.
(författare)
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Estrogen Receptor a Promotes Breast Cancer by Reprogramming Choline Metabolism
- 2016
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Ingår i: Cancer Research. - : AMER ASSOC CANCER RESEARCH. - 0008-5472 .- 1538-7445. ; 76:19, s. 5634-5646
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Tidskriftsartikel (refereegranskat)abstract
- Estrogen receptor alpha (ER alpha) is a key regulator of breast growth and breast cancer development. Here, we report how ER alpha impacts these processes by reprogramming metabolism in malignant breast cells. We employed an integrated approach, combining genome-wide mapping of chromatin-bound ER alpha with estrogeninduced transcript and metabolic profiling, to demonstrate that ER alpha reprograms metabolism upon estrogen stimulation, including changes in aerobic glycolysis, nucleotide and amino acid synthesis, and choline (Cho) metabolism. Cho phosphotransfse CHPT1, identified as a direct era-regulated gene, was required for estrogen- induced effects on Cho metabolism, including increased phosphatidylcholine synthesis. CHPT1 silencing inhibited anchorage- independent growth and cell proliferation, also suppressing early-stage metastasis of tamoxifen-resistant breast cancer cells in a zebrafish xenograft model. Our results showed that era promotes metabolic alterations in breast cancer cells mediated by its target CHPT1, which this study implicates as a candidate therapeutic target. (C) 2016 AACR.
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| 9. |
- Le, Thanh-Tung, et al.
(författare)
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Phosphorus-doped Fe7S8@C nanowires for efficient electrochemical hydrogen and oxygen evolutions: Controlled synthesis and electronic modulation on active sites
- 2021
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Ingår i: Journal of Materials Science & Technology. - : JOURNAL MATER SCI TECHNOL. - 1005-0302. ; 74, s. 168-175
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Tidskriftsartikel (refereegranskat)abstract
- Developing low-cost, efficient, and stable non-precious-metal electrocatalysts with controlled crystal structure, morphology and compositions are highly desirable for hydrogen and oxygen evolution reactions. Herein, a series of phosphorus-doped Fe7S8 nanowires integrated within carbon (P-Fe7S8@C) are rationally synthesized via a one-step phosphorization of one-dimensional (1D) Fe-based organic-inorganic nanowires. The as-obtained P-Fe7S8@C catalysts with modified electronic configurations present typical porous structure, providing plentiful active sites for rapid reaction kinetics. Density functional calculations demonstrate that the doping Fe7S8 with P can effectively enhance the electron density of Fe7S8 around the Fermi level and weaken the Fe-H bonding, leading to the decrease of adsorption free energy barrier on active sites. As a result, the optimal catalyst of P-Fe7S8-600@C exhibits a relatively low overpotential of 136 mV for hydrogen evolution reaction (HER) to reach the current density of 10 mA/cm(2), and a significantly low overpotential of 210 mV for oxygen evolution reaction (OER) at 20 mA/cm(2) in alkaline media. The work presented here may pave the way to design and synthesis of other prominent Fe-based catalysts for water splitting via electronic regulation. (C) 2021 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.
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| 10. |
- Qu, Yanhua, 1974-, et al.
(författare)
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The evolution of ancestral and species-specific adaptations in snowfinches at the Qinghai-Tibet Plateau
- 2021
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Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 10.1073/pnas.2012398118:13, s. e2012398118-e2012398118
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Tidskriftsartikel (refereegranskat)abstract
- Species in a shared environment tend to evolve similar adaptations under the influence of their phylogenetic context. Using snowfinches, a monophyletic group of passerine birds (Passeridae), we study the relative roles of ancestral and species-specific adaptations to an extreme high-elevation environment, the Qinghai–Tibet Plateau. Our ancestral trait reconstruction shows that the ancestral snowfinch occupied high elevations and had a larger body mass than most nonsnowfinches in Passeridae. Subsequently, this phenotypic adaptation diversified in the descendant species. By comparing high-quality genomes from representatives of the three phylogenetic lineages, we find that about 95% of genes under positive selection in the descendant species are different from those in the ancestor. Consistently, the biological functions enriched for these species differ from those of their ancestor to various degrees (semantic similarity values ranging from 0.27 to 0.5), suggesting that the three descendant species have evolved divergently from the initial adaptation in their common ancestor. Using a functional assay to a highly selective gene, DTL, we demonstrate that the nonsynonymous substitutions in the ancestor and descendant species have improved the repair capacity of ultraviolet-induced DNA damage. The repair kinetics of the DTL gene shows a twofold to fourfold variation across the ancestor and the descendants. Collectively, this study reveals an exceptional case of adaptive evolution to high-elevation environments, an evolutionary process with an initial adaptation in the common ancestor followed by adaptive diversification of the descendant species.
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