| 1. |
- Beal, Jacob, et al.
(författare)
-
Robust estimation of bacterial cell count from optical density
- 2020
-
Ingår i: Communications Biology. - : Springer Science and Business Media LLC. - 2399-3642. ; 3:1
-
Tidskriftsartikel (refereegranskat)abstract
- Optical density (OD) is widely used to estimate the density of cells in liquid culture, but cannot be compared between instruments without a standardized calibration protocol and is challenging to relate to actual cell count. We address this with an interlaboratory study comparing three simple, low-cost, and highly accessible OD calibration protocols across 244 laboratories, applied to eight strains of constitutive GFP-expressing E. coli. Based on our results, we recommend calibrating OD to estimated cell count using serial dilution of silica microspheres, which produces highly precise calibration (95.5% of residuals <1.2-fold), is easily assessed for quality control, also assesses instrument effective linear range, and can be combined with fluorescence calibration to obtain units of Molecules of Equivalent Fluorescein (MEFL) per cell, allowing direct comparison and data fusion with flow cytometry measurements: in our study, fluorescence per cell measurements showed only a 1.07-fold mean difference between plate reader and flow cytometry data.
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| 2. |
- Li, Mian, et al.
(författare)
-
Halogenated Ti3C2 MXenes with Electrochemically Active Terminals for High-Performance Zinc Ion Batteries
- 2021
-
Ingår i: ACS Nano. - : AMER CHEMICAL SOC. - 1936-0851 .- 1936-086X. ; 15:1, s. 1077-1085
-
Tidskriftsartikel (refereegranskat)abstract
- The class of two-dimensional metal carbides and nitrides known as MXenes offer a distinct manner of property tailoring for a wide range of applications. The ability to tune the surface chemistry for expanding the property space of MXenes is thus an important topic, although experimental exploration of surface terminals remains a challenge. Here, we synthesized Ti3C2 MXene with unitary, binary, and ternary halogen terminals, e.g., -Cl, -Br, -I, -BrI, and -ClBrI, to investigate the effect of surface chemistry on the properties of MXenes. The electrochemical activity of Br and I elements results in the extraordinary electrochemical performance of the MXenes as cathodes for aqueous zinc ion batteries. The -Br- and -I-containing MXenes, e.g., Ti3C2Br2 and Ti3C2I2, exhibit distinct discharge platforms with considerable capacities of 97.6 and 135 mA.g(-1). Ti3C2 (BrI) and Ti3C2 (ClBrI) exhibit dual discharge platforms with capacities of 117.2 and 106.7 mAh.g(-1). In contrast, the previously discovered MXenes Ti3C2Cl2 and Ti3C2 (OF) exhibit no discharge platforms and only similar to 50% of capacities and energy densities of Ti3C2Br2. These results emphasize the effectiveness of the Lewis-acidic-melt etching route for tuning the surface chemistry of MXenes and also show promise for expanding the MXene family toward various applications.
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| 3. |
- Ding, Haoming, et al.
(författare)
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Chemical scissor-mediated structural editing of layered transition metal carbides
- 2023
-
Ingår i: Science. - : AMER ASSOC ADVANCEMENT SCIENCE. - 0036-8075 .- 1095-9203. ; 379:6637, s. 1130-1135
-
Tidskriftsartikel (refereegranskat)abstract
- Intercalated layered materials offer distinctive properties and serve as precursors for important two-dimensional (2D) materials. However, intercalation of non-van der Waals structures, which can expand the family of 2D materials, is difficult. We report a structural editing protocol for layered carbides (MAX phases) and their 2D derivatives (MXenes). Gap-opening and species-intercalating stages were respectively mediated by chemical scissors and intercalants, which created a large family of MAX phases with unconventional elements and structures, as well as MXenes with versatile terminals. The removal of terminals in MXenes with metal scissors and then the stitching of 2D carbide nanosheets with atom intercalation leads to the reconstruction of MAX phases and a family of metal-intercalated 2D carbides, both of which may drive advances in fields ranging from energy to printed electronics.
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| 4. |
- Ding, Haoming, et al.
(författare)
-
Synthesis of MAX phases Nb2CuC and Ti2(Al0.1Cu0.9)N by A-site replacement reaction in molten salts
- 2019
-
Ingår i: Materials Research Letters. - : Taylor & Francis. - 2166-3831. ; 7:12, s. 510-516
-
Tidskriftsartikel (refereegranskat)abstract
- New MAX phases Ti2(AlxCu1−x)N and Nb2CuC were synthesized by A-site replacement by reacting Ti2AlN and Nb2AlC, respectively, with CuCl2 or CuI molten salt. X-ray diffraction, scanning electron microscopy, and atomically resolved scanning transmission electron microscopy showed complete A-site replacement in Nb2AlC, which lead to the formation of Nb2CuC. However, the replacement of Al in Ti2AlN phase was only close to complete at Ti2(Al0.1Cu0.9)N. Density-functional theory calculations corroborated the structural stability of Nb2CuC and Ti2CuN phases. Moreover, the calculated cleavage energy in these Cu-containing MAX phases are weaker than in their Al-containing counterparts.The preparation of MAX phases Nb2CuC and Ti2(Al0.1Cu0.9)N were realized by A-site replacement in Ti2AlN and Nb2AlN, respectively.
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| 5. |
- Li, Mian, et al.
(författare)
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Element Replacement Approach by Reaction with Lewis Acidic Molten Salts to Synthesize Nanolaminated MAX Phases and MXenes
- 2019
-
Ingår i: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 141:11, s. 4730-4737
-
Tidskriftsartikel (refereegranskat)abstract
- Nanolaminated materials are important because of their exceptional properties and wide range of applications. Here, we demonstrate a general approach to synthesizing a series of Zn-based MAX phases and Cl-terminated MXenes originating from the replacement reaction between the MAX phase and the late transition-metal halides. The approach is a top-down route that enables the late transitional element atom (Zn in the present case) to occupy the A site in the pre-existing MAX phase structure. Using this replacement reaction between the Zn element from molten ZnCl2 and the Al element in MAX phase precursors (Ti3AlC2, Ti2AlC, Ti2AlN, and V2AlC), novel MAX phases Ti3ZnC2, Ti2ZnC, Ti2ZnN, and V2ZnC were synthesized. When employing excess ZnCl2, Cl-terminated MXenes (such as Ti3C2Cl2 and Ti2CCl2) were derived by a subsequent exfoliation of Ti3ZnC2 and Ti2ZnC due to the strong Lewis acidity of molten ZnCl2. These results indicate that A-site element replacement in traditional MAX phases by late transition-metal halides opens the door to explore MAX phases that are not thermodynamically stable at high temperature and would be difficult to synthesize through the commonly employed powder metallurgy approach. In addition, this is the first time that exclusively Cl-terminated MXenes were obtained, and the etching effect of Lewis acid in molten salts provides a green and viable route to preparing MXenes through an HF-free chemical approach.
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| 6. |
- Li, Shiyu, et al.
(författare)
-
Docking and Activity of DNA Polymerase on Solid-State Nanopores
- 2022
-
Ingår i: ACS Sensors. - : American Chemical Society (ACS). - 2379-3694. ; 7:5, s. 1476-1483
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Tidskriftsartikel (refereegranskat)abstract
- Integration of motor enzymes with biological nanopores has enabled commercial DNA sequencing technology; yet studies of the similar principle applying to solid-state nanopores are limited. Here, we demonstrate the real-life monitoring of phi29 DNA polymerase (DNAP) docking onto truncated-pyramidal nanopore (TPP) arrays through both electrical and optical readout. To achieve effective docking, atomic layer deposition of hafnium oxide is employed to reduce the narrowest pore opening size of original silicon (Si) TPPs to sub-10 nm. On a single TPP with pore opening size comparable to DNAP, ionic current measurements show that a polymerase-DNA complex can temporally dock onto the TPP with a certain docking orientation, while the majority become translocation events. On 5-by-5 TPP arrays, a label-free optical detection method using Ca2+ sensitive dye, are employed to detect the docking dynamics of DNAP. The results show that this label-free detection strategy is capable of accessing the docking events of DNAP on TPP arrays. Finally, we examine the activity of docked DNAP by performing on-site rolling circle amplification to synthesize single-stranded DNA (ssDNA), which serves as a proof-of-concept demonstration of utilizing this docking scheme for emerging nanopore sensing applications.
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| 7. |
- Li, Shiyu, et al.
(författare)
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Dynamics of DNA Clogging in Hafnium Oxide Nanopores
- 2020
-
Ingår i: Journal of Physical Chemistry B. - : American Chemical Society (ACS). - 1520-6106 .- 1520-5207. ; 124:51, s. 11573-11583
-
Tidskriftsartikel (refereegranskat)abstract
- Interfacing solid-state nanopores with biological systems has been exploited as a versatile analytical platform for analysis of individual biomolecules. Although clogging of solid-state nanopores due to nonspecific interactions between analytes and pore walls poses a persistent challenge in attaining the anticipated sensing efficacy, insufficient studies focus on elucidating the clogging dynamics. Herein, we investigate the DNA clogging behavior by passing double-stranded (ds) DNA molecules of different lengths through hafnium oxide(HfO2)-coated silicon (Si) nanopore arrays, at different bias voltages and electrolyte pH values. Employing stable and photoluminescent-free HfO2/Si nanopore arrays permits a parallelized visualization of DNA clogging with confocal fluorescence microscopy. We find that the probability of pore clogging increases with both DNA length and bias voltage. Two types of clogging are discerned: persistent and temporary. In the time-resolved analysis, temporary clogging events exhibit a shorter lifetime at higher bias voltage. Furthermore, we show that the surface charge density has a prominent effect on the clogging probability because of electrostatic attraction between the dsDNA and the HfO2 pore walls. An analytical model based on examining the energy landscape along the DNA translocation trajectory is developed to qualitatively evaluate the DNA–pore interaction. Both experimental and theoretical results indicate that the occurrence of clogging is strongly dependent on the configuration of translocating DNA molecules and the electrostatic interaction between DNA and charged pore surface. These findings provide a detailed account of the DNA clogging phenomenon and are of practical interest for DNA sensing based on solid-state nanopores.
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| 8. |
- Li, Shiyu, 1991-
(författare)
-
Engineering Surfaces of Solid-State Nanopores for Biomolecule Sensing
- 2021
-
Konstnärligt arbete (övrigt vetenskapligt/konstnärligt)abstract
- Nanopores have emerged as a special class of single-molecule analytical tool that offers immense potential for sensing and characterizing biomolecules such as nucleic acids and proteins. As an alternative to biological nanopores, solid-state nanopores present remarkable versatility due to their wide-range tunability in pore geometry and dimension as well as their excellent mechanical robustness and stability. However, being intrinsically incompatible with biomolecules, surfaces of inorganic solids need be modified to provide desired functionalities for real-life sensing purposes. In this thesis, we presented an exploration of various surface engineering strategies and an examination of several surface associated phenomena pertaining specifically to solid-state nanopores. Based on the parallel sensing concept using arrayed pores, optical readout is mainly employed throughout the whole study.For the surface engineering aspect, a list of approaches was explored. A versatile surface patterning strategy for immobilization of biomolecules was developed based on selective poly(vinylphosphonic acid) passivation and electron beam induced deposition technique. This scheme was then implemented on nanopore arrays for nanoparticle localization. In addition, vesicle rupture-based lipid bilayer coating was adapted to truncated-pyramidal nanopores, which was shown to be effective for the minimizing DNA-pore interaction. Further, HfO2 coating by means of atomic layer deposition was employed to prevent the erosion of Si-based pores and to shrink the pore diameter, which enabled reliable investigations of DNA clogging and DNA polymerase docking.For the surface associated phenomena, several findings were made. The lipid bilayer formation on truncated pyramidal nanopores via instantaneous rupture of individual vesicles was quantified based on combined ionic current monitoring and optical observation. The probability of pore clogging appeared to linearly increase with the length of DNA strands and applied bias voltage, which could be attributed a higher probability of knotting and/or folding of longer DNA strands and more frequent translocation events at higher voltage. A free-energy based analytical model was proposed to evaluate the DNA-pore interaction and to interpret observed clogging behavior. Finally, docking of DNA polymerase on nanopore arrays was demonstrated using label-free optical method based on Ca2+ indicator dyes, which may open the avenue to sequencing-by-synthesis enabled by the docked polymerase.
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| 9. |
- Li, Shiyu, et al.
(författare)
-
Label-Free Optical Detection of DNA Polymerase Docking on Solid-State Nanopore Arrays
-
Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Integration of motor enzymes with biological nanopores has enabled commercial DNA sequencing, yet studies of the similar principle applying to solid-state nanopores are limited. Here, we demonstrate the label-free optical detection of phi29 DNA polymerase (DNAP) docking onto truncated-pyramidal nanopores (TPP). Atomic layer deposition of hafnium oxide is employed to shrink the pore opening size of original silicon (Si) TPP to sub-10 nm. Ionic current measurements of single TPP of an opening size comparable to DNAP show that polymerase-DNA complexes can temporally dock onto the TPP with a certain docking orientation, while the majority are translocation events. A label-free optical detection method using Ca2+ sensitive dye is employed to detect the docking of DNAP on 5-by-5 nanopore arrays. The results of the proof-of-concept experiment show that this label-free detection strategy is capable of accessing the docking events of DNAP on solid-state nanopore arrays.
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| 10. |
- Li, Shiyu, et al.
(författare)
-
Nanoarrays on Passivated Aluminum Surface for Site-Specific Immobilization of Biomolecules
- 2018
-
Ingår i: ACS Applied Bio Materials. - : American Chemical Society (ACS). - 2576-6422. ; 1:1, s. 125-135
-
Tidskriftsartikel (refereegranskat)abstract
- The rapid development of biosensing platforms for highly sensitive and specific detection raises the desire of precise localization of biomolecules onto various material surfaces. Aluminum has been strategically employed in the biosensor system due to its compatibility with CMOS technology and its optical and electrical properties such as prominent propagation of surface plasmons. Herein, we present an adaptable method for preparation of carbon nanoarrays on aluminum surface passivated with poly(vinylphosphonic acid) (PVPA). The carbon nanoarrays were defined by means of electron beam induced deposition (EBID) and they were employed to realize site-specific immobilization of target biomolecules. To demonstrate the concept, selective streptavidin/neutravidin immobilization on the carbon nanoarrays was achieved through protein physisorption with a significantly high contrast of the carbon domains over the surrounding PVPA-modified aluminum surface. By adjusting the fabrication parameters, local protein densities could be varied on similarly sized nanodomains in a parallel process. Moreover, localization of single 40 nm biotinylated beads was achieved by loading them on the neutravidin-decorated nanoarrays. As a further demonstration, DNA polymerase with a streptavidin tag was bound to the biotin-beads that were immobilized on the nanoarrays and in situ rolling circle amplification (RCA) was subsequently performed. The observation of organized DNA arrays synthesized by RCA verified the nanoscale localization of the enzyme with retained biological activity. Hence, the presented approach could provide a flexible and universal avenue to precise localizing various biomolecules on aluminum surface for potential biosensor and bioelectronic applications.
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| 11. |
- Li, Shiyu, et al.
(författare)
-
Nanoparticle Localization on Solid-State Nanopores Via Electrophoretic Force
- 2019
-
Ingår i: 2019 20TH INTERNATIONAL CONFERENCE ON SOLID-STATE SENSORS, ACTUATORS AND MICROSYSTEMS & EUROSENSORS XXXIII (TRANSDUCERS & EUROSENSORS XXXIII). - : IEEE. - 9781728120072 ; , s. 2372-2375
-
Konferensbidrag (refereegranskat)abstract
- This work presents a versatile and facile method for precise localization of nanoparticles on solid-state nanopores surface-functionalized with carbon via electron beam induced deposition (EBID). For the first time, EBID of carbon is demonstrated to enable nanoparticle localization on solid-state nanopores. To avoid non-specific adsorption of nanoparticles on the surface, an atomic layer deposited Al2O3 layer in combination with phosphonate passivation is used. By tuning the electron dose in the EBID process, the loading fraction of nanoparticles on carbon nanoarrays can be varied on similarly sized domains. Nanoparticle loading driven by electrophoresis can achieve an efficiency that is orders of magnitude higher than that driven by diffusion.
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| 12. |
- Li, Shiyu, et al.
(författare)
-
Visualization of DNA Translocation and Clogging Using Photoluminescent-Free Silicon Nanopore Arrays
- 2020
-
Ingår i: 2020 IEEE 20th International Conference on Nanotechnology (IEEE-NANO). - : Institute of Electrical and Electronics Engineers (IEEE). - 9781728182643 ; , s. 193-197
-
Konferensbidrag (refereegranskat)abstract
- Solid-state nanopore arrays hold promises for high-throughput optical analysis of single molecules. However, the high photoluminescence (PL) background emanating from the commonly used silicon nitride (SiNx) membrane for nanopore fabrication and the nonspecific adsorption of analyte on the pore sidewalls have plagued the high sensing sensitivity and efficiency offered by optical sensing. Here, the present work demonstrates an optical monitoring system using a truncated pyramidal nanopore array on a silicon membrane coated with a lipid bilayer for visualization of DNA translocation events. The silicon membrane produces essentially no PL under blue-green laser illumination, which enables more clear identification of DNA translocation and clogging events than using SiNx-based devices. The lipid bilayer coating based on small unilamellar vesicles (SUVs) minimizes the nonspecific adsorption of DNA. With confocal microscopy, the fluorescent labeled DNA translocation motion is visualized in three dimensions. The statistical results show that the percentage of DNA clogged pores is significantly reduced for the lipid bilayer coated nanopores as compared to the uncoated nanopores.
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| 13. |
- Li, Youbing, et al.
(författare)
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A general Lewis acidic etching route for preparing MXenes with enhanced electrochemical performance in non-aqueous electrolyte
- 2020
-
Ingår i: Nature Materials. - : NATURE PUBLISHING GROUP. - 1476-1122 .- 1476-4660. ; 19:8, s. 894-899
-
Tidskriftsartikel (refereegranskat)abstract
- Two-dimensional transition metal carbides and nitrides, known as MXenes, are currently considered as energy storage materials. A generic Lewis acidic etching route for preparing high-rate negative-electrode MXenes with enhanced electrochemical performance in non-aqueous electrolyte is now proposed. Two-dimensional carbides and nitrides of transition metals, known as MXenes, are a fast-growing family of materials that have attracted attention as energy storage materials. MXenes are mainly prepared from Al-containing MAX phases (where A = Al) by Al dissolution in F-containing solution; most other MAX phases have not been explored. Here a redox-controlled A-site etching of MAX phases in Lewis acidic melts is proposed and validated by the synthesis of various MXenes from unconventional MAX-phase precursors with A elements Si, Zn and Ga. A negative electrode of Ti3C2 MXene material obtained through this molten salt synthesis method delivers a Li+ storage capacity of up to 738 C g(-1) (205 mAh g(-1)) with high charge-discharge rate and a pseudocapacitive-like electrochemical signature in 1 M LiPF6 carbonate-based electrolyte. MXenes prepared via this molten salt synthesis route may prove suitable for use as high-rate negative-electrode materials for electrochemical energy storage applications.
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| 14. |
- Li, Youbing, et al.
(författare)
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A-site alloying-guided universal design of noble metal-based MAX phases
- 2024
-
Ingår i: Matter. - : Cell Press. - 2590-2393 .- 2590-2385. ; 7:2, s. 523-538
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Tidskriftsartikel (refereegranskat)abstract
- Mn+1AXn (MAX) phases have attracted significant attention due to their structural diversity and potential applications. Designing MAX phases with single-atom-thick A layers featuring 4d/5d-orbital electronic elements is interesting work. Here, we present a comprehensive report on noble metal-based M2(A1-xA′x)C (M = V, Ti, Nb; A = Al, Sn, In, Ga, Ge; A′ = Ru, Rh, Pd, Ir, Pt, Au and combinations thereof; 0 < x ≤ 0.4) phases featuring A sublayers of 4d/5d-orbital electronic elements through an A-site alloying strategy. The chemical composition of MAX phases can be adjusted by selecting different M- and A-site elements, with morphology tailored by distinct C sources. Furthermore, the V2(Sn0.8Pt0.2)C (15.7 wt % Pt) catalyst showed better performance for hydrogen evolution reaction compared to the commercial Pt/C (20 wt % Pt) electrode. This study highlights the prospects of A-site alloying for the design of novel MAX phases with unique properties and promising applications in electrocatalysis and beyond.
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| 15. |
- Li, Youbing, et al.
(författare)
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Electrochemical Lithium Storage Performance of Molten Salt Derived V2SnC MAX Phase
- 2021
-
Ingår i: Nano-Micro Letters. - : Springer. - 2311-6706 .- 2150-5551. ; 13:1
-
Tidskriftsartikel (refereegranskat)abstract
- MAX phases are gaining attention as precursors of two-dimensional MXenes that are intensively pursued in applications for electrochemical energy storage. Here, we report the preparation of V2SnC MAX phase by the molten salt method. V2SnC is investigated as a lithium storage anode, showing a high gravimetric capacity of 490 mAh g(-1) and volumetric capacity of 570 mAh cm(-3) as well as superior rate performance of 95 mAh g(-1) (110 mAh cm(-3)) at 50 C, surpassing the ever-reported performance of MAX phase anodes. Supported by operando X-ray diffraction and density functional theory, a charge storage mechanism with dual redox reaction is proposed with a Sn-Li (de)alloying reaction that occurs at the edge sites of V2SnC particles where Sn atoms are exposed to the electrolyte followed by a redox reaction that occurs at V2C layers with Li. This study offers promise of using MAX phases with M-site and A-site elements that are redox active as high-rate lithium storage materials.
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| 16. |
- Li, Youbing, et al.
(författare)
-
Multielemental single atom-thick A layers in nanolaminated V2(Sn, A) C (A = Fe, Co, Ni, Mn) for tailoring magnetic properties
- 2020
-
Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : NATL ACAD SCIENCES. - 0027-8424 .- 1091-6490. ; 117:2, s. 820-825
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Tidskriftsartikel (refereegranskat)abstract
- Tailoring of individual single-atom-thick layers in nanolaminated materials offers atomic-level control over material properties. Nonetheless, multielement alloying in individual atomic layers in nanolaminates is largely unexplored. Here, we report 15 inherently nanolaminated V-2(A(x)Sn(1-x))C (A = Fe, Co, Ni, Mn, and combinations thereof, with x similar to 1/3) MAX phases synthesized by an alloy-guided reaction. The simultaneous occupancy of the 4 magnetic elements and Sn in the individual single-atom-thick A layers constitutes high-entropy MAX phase in which multielemental alloying exclusively occurs in the 2 -dimensional (2D) A layers. V-2(A(x)Sn(1-x))C exhibit distinct ferromagnetic behavior that can be compositionally tailored from the multielement A-layer alloying. Density functional theory and phase diagram calculations are performed to understand the structure stability of these MAX phases. This 2D multielemental alloying approach provides a structural design route to discover nanolaminated materials and expand their chemical and physical properties. In fact, the magnetic behavior of these multielemental MAX phases shows strong dependency on the combination of various elements.
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| 17. |
- Li, Youbing, et al.
(författare)
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Nanolaminated Ternary Transition Metal Carbide (MAX Phase)-Derived Core-Shell Structure Electrocatalysts for Hydrogen Evolution and Oxygen Evolution Reactions in Alkaline Electrolytes
- 2023
-
Ingår i: The Journal of Physical Chemistry Letters. - : AMER CHEMICAL SOC. - 1948-7185. ; 14:2, s. 481-488
-
Tidskriftsartikel (refereegranskat)abstract
- The development of abundant, cheap, and highly active catalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is important for hydrogen production. Nanolaminate ternary transition metal carbides (MAX phases) and their derived two-dimensional transition metal carbides (MXenes) have attracted considerable interest for electrocatalyst applications. Herein, four new MAX@MXene core-shell structures (Ta2CoC@ Ta2CTx, Ta2NiC@Ta2CTx, Nb2CoC@Nb2CTx, and Nb2NiC@Nb2CTx), in which the core region is Co/Ni-MAX phases while the edge region is MXenes, have been prepared. Under alkaline electrolyte conditions, the Ta2CoC@Ta2CTx core-shell structure showed an overpotential of 239 mV and excellent stability during the HER with MXenes as the active sites. For the OER, the Ta2CoC@Ta2CTx core- shell structure showed an overpotential of 373 mV and a small Tafel plot (56 mV dec-1), which maintained a bulk crystalline structure and generated Co-based oxyhydroxides that formed by surface reconstruction as active sites. Considering rich chemical compositions and structures of MAX phases, this work provides a new strategy for designing multifunctional electrocatalysts and also paves the way for further development of MAX phase-based materials for clean energy applications.
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| 18. |
- Li, Youbing, et al.
(författare)
-
Near-room temperature ferromagnetic behavior of single-atom-thick 2D iron in nanolaminated ternary MAX phases
- 2021
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Ingår i: Applied Physics Reviews. - : AIP Publishing. - 1931-9401. ; 8:3
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Tidskriftsartikel (refereegranskat)abstract
- M(n+)(1)AX(n) (MAX) phases nanolaminated ternary carbides or nitrides possess a unique crystal structure in which single-atom-thick "A" sublayers are interleaved by alternative stacking of a "Mn+1Xn" sublayer; these materials have been investigated as promising high-safety structural materials for industrial applications because of their laminated structure and metal and ceramic properties. However, limited of A-site elements in the definition of M(n+)(1)AX(n) phases, it is a huge challenge for designing nanolaminated ferromagnetic materials with single-atom-thick two-dimensional iron layers occupying the A layers in the M(n+)(1)AX(n) phases. Here, we report three new ternary magnetic M(n+)(1)AX(n) phases (Ta2FeC, Ti2FeN, and Nb2FeC) with A sublayers of single-atom-thick two-dimensional iron through an isomorphous replacement reaction of M(n+)(1)AX(n) precursors (Ta2AlC, Ti2AlN, and Nb2AlC) with a Lewis acid salts (FeCl2). All these M(n+)(1)AX(n) phases exhibit ferromagnetic behavior. The Curie temperatures of the Ta2FeC and Nb2FeC M(n+)(1)AX(n) phases are 281 and 291K, respectively, i.e., close to room temperature. The saturation magnetization of these ternary magnetic MAX phases is almost two orders of magnitude higher than V-2(Sn,Fe)C, whose A-site is partially substituted by Fe. Theoretical calculations on magnetic orderings of spin moments of Fe atoms in these nanolaminated magnetic M(n+)(1)AX(n) phases reveal that the magnetism can be mainly ascribed to an intralayer exchange interaction of the two-dimensional Fe atomic layers. Owing to the richness in composition of M(n+)(1)AX(n) phases, our work provides a large imaginary space for constructing functional single-atom-thick two-dimensional layers in materials using these nanolaminated templates.
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| 19. |
- Li, Youbing, et al.
(författare)
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Single-Atom-Thick Active Layers Realized in Nanolaminated Ti-3(AlxCu1-x)C-2 and Its Artificial Enzyme Behavior
- 2019
-
Ingår i: ACS Nano. - : AMER CHEMICAL SOC. - 1936-0851 .- 1936-086X. ; 13:8, s. 9198-9205
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Tidskriftsartikel (refereegranskat)abstract
- A Ti-3(AlxCu1-x)C-2 phase with Cu atoms with a degree of ordering in the A plane is synthesized through the A site replacement reaction in CuCl2 molten salt. The weakly bonded single -atom -thick Cu layers in a Ti-3(AlxCu1-x)C-2 MAX phase provide actives sites for catalysis chemistry. As -synthesized Ti-3(AlxCu1-x)C-2 presents unusual peroxidase-like catalytic activity similar to that of natural enzymes. A fabricated Ti-3(AlxCu1-x)C-2/chitosan/glassy carbon electrode biosensor prototype also exhibits a low detection limit in the electrochemical sensing of H2O2. These results have broad implications for property tailoring in a nanolaminated MAX phase by replacing the A site with late transition elements.
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| 20. |
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Optical monitoring of single nanoparticle capture in solid-state nanopore array
- 2019
-
Proceedings (redaktörskap) (refereegranskat)abstract
- Solid-state nanopore arrays hold promises for high-throughput optical or electrical analysis of nanoscale entities. Here, we demonstrate an optical monitoring system for investigation of the capture process of single nanoparticles driven by electrophoretic force in a nanopore array. Over 50% of the single nanoparticle capture events are achieved by controlling the applied voltage across the nanopore membrane with a tailored nanopore size. We find that at a certain voltage bias, the capture of single nanoparticles is a self-termination process.
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| 21. |
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Parallelized single-molecule translocations in arrayed silicon nanopores coated with a lipid bilayer
- 2019
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Proceedings (redaktörskap) (refereegranskat)abstract
- Solid-state nanopores have been recognized as a versatile tool for single-molecule detection with high sensitivity. They have been extensively studied for analysis by nanopore translocation of biomolecules, such as DNA, RNA, and proteins. As a complement to the electrical sensing readout, optical sensing of labeled molecules on a solid-state nanopore array can notably enhance the sensing capacity with high throughput. However, the widely used silicon nitride (SiNx) nanopore produces significant photoluminescence (PL) background under blue-green laser illumination, which can severely limit, e.g., multicolor sensing for DNA barcode discrimination. In addition, the occasionally occurring irreversible DNA clogging in a solid-state nanopore, because of DNA molecules interacting with the nanopore channel wall during translocation, can seriously affect the sensing efficacy and accuracy. To address these problems, we have developed an optical sensing system dedicated to nanopore arrays fabricated in a free-standing silicon membrane with its surface functionalized by lipid bilayer coating.A silicon nanopore array with pores of sub-20 nm diameter is fabricated in a silicon-on-insulator wafer using electron beam lithography in combination with anisotropic etching. The 55 nm thick free-standing silicon membrane shows negligible PL emission in the 550 to 800 nm spectral range under blue-green laser illumination, which greatly improves the optical signal-to-background ratio for single-molecule detection in comparison with standard SiNx devices. The formation of a lipid bilayer on the nanopore walls is successful as inferred by monitoring in situ the stepwise reduction of the nanopore conductance of ionic current and subsequently by observing ex situ the homogenous fluorescence emitted from a labeled lipid bilayer. As a demonstration, we perform the optical sensing measurements with a conventional wide-field microscope to detect the translocation of fluorophore-labeled DNA strands (120 kbp). With the low background PL of the silicon membrane, the optical signal of individual DNA translocation events is more clearly identified than when using similarly processed SiNx nanopore devices. Moreover, the coated fluidic lipid bilayer provides a nonstick surface to minimize the non-specific interaction of DNA molecules with the silicon pore walls. The results show that the DNA clogging is substantially reduced in the lipid bilayer coated nanopores as compared to uncoated nanopores. These results demonstrate that using silicon nanopores coated by a lipid bilayer is a promising strategy to realizing massively-parallel single-molecule optical detection.
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| 22. |
- Pham, Ngan Hoang, et al.
(författare)
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Self-Limited Formation of Bowl-Shaped Nanopores for Directional DNA Translocation
- 2021
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 15:11, s. 17938-17946
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Tidskriftsartikel (refereegranskat)abstract
- Solid-state nanopores of on-demand dimensions and shapes can facilitate desired sensor functions. However, reproducible fabrication of arrayed nanopores of predefined dimensions remains challenging despite numerous techniques explored. Here, bowl-shaped nanopores combining properties of ultrathin membrane and tapering geometry are manufactured using a self-limiting process developed on the basis of standard silicon technology. The upper opening of the bowl-nanopores is 60–120 nm in diameter, and the bottom orifice reaches sub-5 nm. Current-voltage characteristics of the fabricated bowl-nanopores display insignificant rectification indicating weak ionic selectivity, in accordance to numerical simulations showing minor differences in electric field and ionic velocity upon the reversal of bias voltages. Simulations reveal, concomitantly, high-momentum electroosmotic flow downward along the concave nanopore sidewall. Collisions between the left and right tributaries over the bottom orifice drive the electroosmotic flow both up into the nanopore and down out of the nanopore through the orifice. The resultant asymmetry in electrophoretic–electroosmotic force is considered the cause responsible for the experimentally observed strong directionality in λ-DNA translocation with larger amplitude, longer duration, and higher frequencies for the downward movements from the upper opening than the upward ones from the orifice. Thus, the resourceful silicon nanofabrication technology is shown to enable nanopore designs toward enriching sensor applications.
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| 23. |
- Wen, Chenyu, et al.
(författare)
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Autogenic analyte translocation in nanopores
- 2019
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Ingår i: Nano Energy. - : Elsevier. - 2211-2855 .- 2211-3282. ; 60, s. 503-509
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Tidskriftsartikel (refereegranskat)abstract
- Nanopores have been widely studied for power generation and single-molecule detection. Although the power level generated by a single nanopore based on electrolyte concentration gradient is too low to be practically useful, such a power level is found sufficient to drive analyte translocation in nanopores. Here, we explore the simultaneous action of a solid-state nanopore as a nanopower generator and a nanoscale biosensor by exploiting the extremely small power generated to drive the analyte translocation in the same nanopore device. This autogenic analyte translocation is demonstrated using protein and DNA for their distinct shape, size and charge. The simple device structure allows for easy implementation of either electrical or optical readout. The obtained nanopore translocation is characterized by typical behaviors expected for an ordinary nanopore sensor powered by an external source. Extensive numerical simulation confirms the power generation and power level generated. It also reveals the fundamentals of autogenic translocation. As it requires no external power source, the sensing can be conducted with simple readout electronics and may allow for integration of high-density nanopores. Our approach demonstrated in this work may pave the way to practical high-throughput single-molecule nanopore sensing powered by the distributed energy harvested by the nanopores themselves.
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| 24. |
- Wen, Chenyu, et al.
(författare)
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On rectification of ionic current in nanopores
- 2019
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Ingår i: Analytical Chemistry. - : American Chemical Society (ACS). - 0003-2700 .- 1520-6882. ; 91:22, s. 14597-14604
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Tidskriftsartikel (refereegranskat)
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| 25. |
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| 26. |
- Zeng, Shuangshuang, et al.
(författare)
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Controlled size reduction and its underlying mechanism to form solid-state nanopores via electron beam induced carbon deposition
- 2019
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Ingår i: Nanotechnology. - : IOP PUBLISHING LTD. - 0957-4484 .- 1361-6528. ; 30:45
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Tidskriftsartikel (refereegranskat)abstract
- Solid-state nanopores have drawn considerable attention for their potential applications in DNA sequencing and nanoparticle analysis. However, fabrication of nanopores, especially those of diameter below 30 nm, requires sophisticated techniques. Here, a versatile method to controllably reduce the diameter of prefabricated large-size pores down to sub-30 nm without greatly increasing the effective pore depth from the original membrane thickness is shown. This method exploits carbon deposition achieved via hydrocarbon evaporation, induced by an incident beam of electrons, and subsequent dissociation of hydrocarbon to solid carbon deposits. The carbon deposition employs a conventional scanning electron microscope equipped with direct visual feedback, along with a stable hydrocarbon source nearby the sample. This work systematically studies how electron beam accelerating voltage, imaging magnification, initial pore size and membrane composition affect the process of pore size reduction. Secondary electrons generated in the membrane material are confirmed to be the main cause of the dissociation of hydrocarbon. Thicker carbon deposited on one side than on the other of the membrane results in an asymmetric nanopore shape and a rectifying ionic transport. A physico-phenomenological model combined with Monte Carlo simulations is proposed to account for the observed carbon deposition behaviors.
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| 27. |
- Zeng, Shuangshuang, et al.
(författare)
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Mechanism and kinetics of lipid bilayer formation in solid-state nanopores
- 2020
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Ingår i: Langmuir. - : American Chemical Society (ACS). - 0743-7463 .- 1520-5827. ; 36:6, s. 1446-1453
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Tidskriftsartikel (refereegranskat)abstract
- Solid-state nanopores provide a highly versatile platform for rapid electrical detection and analysis of single molecules. Lipid bilayer coating of the nanopores can reduce nonspecific analyte adsorption to the nanopore sidewalls and increase the sensing selectivity by providing possibilities for tethering specific ligands in a cell-membrane mimicking environment. However, the mechanism and kinetics of lipid bilayer formation from vesicles remain unclear in the presence of nanopores. In this work, we used a silicon-based, truncated pyramidal nanopore array as the support for lipid bilayer formation. Lipid bilayer formation in the nanopores was monitored in real time by the change in ionic current through the nanopores. Statistical analysis revealed that a lipid bilayer is formed from the instantaneous rupture of individual vesicle upon adsorption in the nanopores, differing from the generally agreed mechanism that lipid bilayer forms at a high vesicle surface coverage on a planar support. The dependence of the lipid bilayer formation process on the applied bias, vesicle size, and concentration was systematically studied. In addition, the nonfouling properties of the lipid bilayer coated nanopores were demonstrated during long single-stranded DNA translocation through the nanopore array. The findings indicate that the lipid bilayer formation process can be modulated by introducing nanocavities intentionally on the planar surface to create active sites or changing the vesicle size and concentration.
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| 28. |
- Chen, Hongxia, et al.
(författare)
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PRL2 Phosphatase Promotes Oncogenic KIT Signaling in Leukemia Cells through Modulating CBL Phosphorylation
- 2024
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Ingår i: Molecular Cancer Research. - 1541-7786. ; 22:1, s. 94-103
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Tidskriftsartikel (refereegranskat)abstract
- Receptor tyrosine kinase KIT is frequently activated in acute myeloid leukemia (AML). While high PRL2 (PTP4A2) expression is correlated with activation of SCF/KIT signaling in AML, the underlying mechanisms are not fully understood. We discovered that inhibition of PRL2 significantly reduces the burden of oncogenic KIT-driven leukemia and extends leukemic mice survival. PRL2 enhances oncogenic KIT signaling in leukemia cells, promoting their proliferation and survival. We found that PRL2 dephosphorylates CBL at tyrosine 371 and inhibits its activity toward KIT, leading to decreased KIT ubiquitination and enhanced AKT and ERK signaling in leukemia cells.
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| 29. |
- Huang, Meng, et al.
(författare)
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Continuous-wave Raman amplification in silicon core fibers pumped in the telecom band
- 2021
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Ingår i: APL PHOTONICS. - : AIP Publishing. - 2378-0967. ; 6:9, s. 096105-
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Tidskriftsartikel (refereegranskat)abstract
- Stimulated Raman amplification is observed for the first time in the silicon core fiber (SCF) platform. The SCFs were tapered to obtain sub-micrometer core dimensions and low optical transmission losses, facilitating efficient spontaneous scattering and stimulated Raman amplification using a continuous-wave pump source with milliwatt power levels. A maximum on-off gain of 1.1 dB was recorded at a pump power of only 48 mW with our numerical simulations, indicating that gains up to 6dB are achievable by increasing the fiber length. This work shows that the SCF platform could open a route to producing compact and robust all-fiber integrated Raman amplifiers and lasers across a broad wavelength region.
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| 30. |
- Huang, Shiyu, et al.
(författare)
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Single-Atom Metal Sites Anchored Hydrogen-Bonded Organic Frameworks for Superior “Two-In-One” Photocatalytic Reaction
- 2023
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Ingår i: Advanced Functional Materials. - : Wiley. - 1616-301X .- 1616-3028. ; 33:21
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Tidskriftsartikel (refereegranskat)abstract
- Photoredox catalysis is a green solution for organics transformation and CO2 conversion into valuable fuels, meeting the challenges of sustainable energy and environmental concerns. However, the regulation of single-atomic active sites in organic framework not only influences the photoredox performance, but also limits the understanding of the relationship for photocatalytic selective organic conversion with CO2 valorization into one reaction system. As a prototype, different single-atomic metal (M) sites (M2+ = Fe2+, Co2+, Ni2+, Cu2+, and Zn2+) in hydrogen-bonded organic frameworks (M-HOF) backbone with bridging structure of metal-nitrogen are constructed by a typical “two-in-one” strategy for superior photocatalytic C-N coupling reactions integrated with CO2 valorization. Remarkably, Zn-HOF achieves 100% conversion of benzylamine oxidative coupling reactions, 91% selectivity of N-benzylidenebenzylamine and CO2 conversion in one photoredox cycle. From X-ray absorption fine structure analysis and density functional theory calculations, the superior photocatalytic performance is attributed to synergic effect of atomically dispersed metal sites and HOF host, decreasing the reaction energy barriers, enhancing CO2 adsorption and forming benzylcarbamic acid intermediate to promote the redox recycle. This work not only affords the rational design strategy of single-atom active sites in functional HOF, but also facilitates the fundamental insights upon the mechanism of versatile photoredox coupling reaction systems.
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| 31. |
- Larsen, Jes K, et al.
(författare)
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Surface modification through air annealing Cu2ZnSn(S,Se)4 absorbers
- 2017
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Ingår i: Thin Solid Films. - : Elsevier BV. - 0040-6090 .- 1879-2731. ; 633, s. 118-121
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Tidskriftsartikel (refereegranskat)abstract
- Recent studies demonstrate that air annealing can have a positive effect on the device performance of Cu2ZnSn(SxSe1-x)(4)[CZTSSe] solar cells. In this work air annealing of the selenium containing CZTSSe is compared to the pure sulfide CZTS. It is discovered that the selenium containing absorbers benefit from air annealing at higher temperatures than selenium free absorbers. The highest efficiency obtained utilizing the air annealing treatment on selenium containing absorbers is 9.7%. We find that the band gap is narrowed when air annealing, which is partially explained by increased Cu-Zn disorder. Furthermore Zn enrichment of the surface after etching is identified as a possible cause of enhanced device performance. It is additionally observed that elemental selenium present on the CZTSSe surface is reduced in the air annealing treatment. Selenium removal is another possible explanation for the enhanced performance caused by the air annealing treatment.
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| 32. |
- Lei, Chengan, et al.
(författare)
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Controllable dual-polarization valley physics in the strain-engineered 2D monolayer of VC2N4
- 2024
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Ingår i: Journal of Materials Chemistry C. - : Royal Society of Chemistry. - 2050-7526 .- 2050-7534. ; 12:6, s. 2156-2164
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Tidskriftsartikel (refereegranskat)abstract
- Valley-related physics has garnered significant attention in fundamental studies and cutting-edge information technologies. However, such valleytronic materials have rarely been reported and suffer from in-plane magnetization. Herein, based on first-principles calculations and tight-binding model analysis, we identify the existence of intrinsic valley-contrasting physics in bipolar ferromagnetic monolayer VC2N4 with robust perpendicular magnetic anisotropy behavior. Valley polarization arises spontaneously due to the simultaneous presence of broken space- and time-inversion symmetries. Interestingly, valley polarization is remarkably observed in both the valence and conduction bands around the K/K′ valley due to large spin splitting, indicating rare dual-polarization valley features, which is advantageous for achieving the captivating anomalous valley Hall effect relied on the valley-contrasting Berry curvature. Remarkably, the valley polarization can be switched on/off by applying a moderate biaxial strain. Our work provides a competitive candidate for exploring valley-dependent physics and its applications in valleytronics.
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| 33. |
- Li, Zhuwei, et al.
(författare)
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Engineering single-atom active sites anchored covalent organic frameworks for efficient metallaphotoredox C-N cross-coupling reactions
- 2022
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Ingår i: Science Bulletin. - : Elsevier BV. - 2095-9273. ; 67:19, s. 1971-1981
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Tidskriftsartikel (refereegranskat)abstract
- Photoredox catalysis has become an indispensable solution for the synthesis of small organic molecules. However, the precise construction of single-atomic active sites not only determines the catalytic performance, but also avails the understanding of structure-activity relationship. Herein, we develop a facile approach to immobilize single-atom Ni sites anchored porous covalent organic framework (COF) by use of 4,40,400-(1,3,5-triazine-2,4,6-triyl)trianiline and 2,6-diformylpyridine (Ni SAS/TD-COF). Ni SAS/TDCOF catalyst achieves excellent catalytic performance in visible-light-driven catalytic carbon-nitrogen cross-coupling reaction between aryl bromides and amines under mild conditions. The reaction provides amine products in excellent yields (71%-97%) with a wide range of substrates, including aryl and heteroaryl bromides with electron-deficient, electron-rich and neutral groups. Notably, Ni SAS/TD-COF could be recovered from the reaction mixture, corresponding to the negligible loss of photoredox performance after several cycles. This work provides a promising opportunity upon rational design of single-atomic active sites on COFs and the fundamental insight of photoredox mechanism for sustainable organic transformation.
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| 34. |
- Li, Zhuwei, et al.
(författare)
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Integrated nickel/polymer dual catalytic system for visible-light-driven sulfonamidation between aryl halides and aryl sulfonamides
- 2022
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Ingår i: CHEM CATALYSIS. - : Elsevier BV. - 2667-1093. ; 2:12, s. 3546-3558
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Tidskriftsartikel (refereegranskat)abstract
- By merging transition metal and heterogeneous photocatalyst, a metal-photoredox system has attracted more attention for cross -coupling of various dual photoredox catalysis. However, there is a grand challenge for the attenuated nucleophilicity of sulfonamides relative to alkyl amines. Herein, an integrated dual catalytic system of porous carbon nitride nanosheet with nitrogen vacancies (NV-P-C3N4)as a conjugated polymer semiconductor host in combination with transition-metal nickel (Ni) was constructed by a defect and morphology regulation strategy toward visible-light-driven sulfona-midation between aryl halides and aryl sulfonamides. The excellent nickel/photoredox-catalyzed C-N coupling reaction performance is ascribed to the large specific surface area, abundant active sites, long carrier lifetime, and efficient transfer and separation of photo -excited electrons and holes. This work highlights the opportunity to cooperate with heterogeneous catalysts and active metal sites for challenging cross-coupling reactions.
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| 35. |
- Si, Xiaoyang, et al.
(författare)
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Effect of carbide interlayers on the microstructure and properties of graphene-nanoplatelet-reinforced copper matrix composites
- 2017
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Ingår i: Materials Science & Engineering. - : ELSEVIER SCIENCE SA. - 0921-5093 .- 1873-4936. ; 708, s. 311-318
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Tidskriftsartikel (refereegranskat)abstract
- Copper matrix composites reinforced with carbide-coated graphene nanoplatelets (GNPs) were investigated in order to understand the role of the interlayers on the thermal, electrical, mechanical and electro-tribological properties of the composites. The TiC or VC coatings were formed in situ on the two sides of GNPs through a controllable reaction in molten salts. Compared with bare GNPs composites, the bonding between the GNPs and copper was improved. Accordingly, the tensile strength and the fracture elongation of Cu/GNPs composites with an interlayer were enhanced by strengthened interfacial bonding. Furthermore, the wear resistance of Cu/GNPs composites was remarkably improved.
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| 36. |
- Wu, Dong, et al.
(författare)
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Four-Wave Mixing-Based Wavelength Conversion and Parametric Amplification in Submicron Silicon Core Fibers
- 2021
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Ingår i: IEEE Journal of Selected Topics in Quantum Electronics. - : Institute of Electrical and Electronics Engineers (IEEE). - 1077-260X .- 1558-4542. ; 27:2
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Tidskriftsartikel (refereegranskat)abstract
- Silicon core fibers represent a versatile platform for all-fiber integrated nonlinear optical applications. This paper describes the state of the art in four-wave mixing-based parametric amplification, and wavelength conversion in silicon fibers that have been tapered to improve the material quality, and engineer the dispersion profile. Fibers with submicron core dimensions have been fabricated, and used to demonstrate high gain parametric amplification in the C-Band, and broadband wavelength conversion extending out to the S-, and L-bands. The potential to use these fibers for all-optical signal processing of 20 Gbit/s data signals has also been demonstrated, with a robust all-fiber coupling scheme presented to improve the efficiency, and practicality of these devices. These results highlight the potential of silicon core fibers for use in nonlinear signal processing within future telecommunication systems.
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| 37. |
- Xu, Xingxing, et al.
(författare)
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Estimating Detection Limits of Potentiometric DNA sensors Using Surface Plasmon Resonance Analyses
- 2020
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Ingår i: ACS Sensors. - : American Chemical Society (ACS). - 2379-3694. ; 5:1, s. 217-224
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Tidskriftsartikel (refereegranskat)abstract
- As the signals of potentiometric-based DNA ion-selective field effect transistor (ISFET) sensors differ largely from report to report, a systematic revisit to this method is needed. Herein, the hybridization of the target and the probe DNA on the sensor surface and its dependence on the surface probe DNA coverage and the ionic strength were systematically investigated by surface plasmon resonance (SPR). The maximum potentiometric DNA hybridization signal that could be registered by an ISFET sensor was estimated based on the SPR measurements, without considering buffering effects from any side interaction on the sensing electrode. We found that under physiological solutions (200 to 300 mM ionic strength), the ISFET sensor could not register the DNA hybridization events on the sensor surface due to Debye screening. Lowering the salt concentration to enlarge the Debye length would at the same time reduce the surface hybridization efficiency, thus suppressing the signal. This adverse effect of low salt concentration on the hybridization efficiency was also found to be more significant on the surface with higher probe coverage due to steric hindrance. With the method of diluting buffer, the maximum potentiometric signal generated by the DNA hybridization was estimated to be only around 120 mV with the lowest detection limit of 30 nM, occurring on a surface with optimized probe coverage and in the tris buffer with 10 mM NaCl. An alternative method would be to achieve high-efficiency hybridization in the buffer with high salt concentration (1 M NaCl) and then to perform potentiometric measurements in the buffer with low salt concentration (1 mM NaCl). Based on the characterization of the stability of the hybridized DNA duplexes on the sensor surface in low salt concentration buffer solutions, the estimated maximum potentiometric signal could be significantly higher using the alternative method. The lowest detection limit for this alternative method was estimated to be around 0.6 nM. This work can serve as an important quantitative reference for potentiometric DNA sensors.
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| 38. |
- Yao, Jia, et al.
(författare)
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Fluorinated Perylene-Diimides: Cathode Interlayers Facilitating Carrier Collection for High-Performance Organic Solar Cells
- 2022
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Ingår i: Advanced Materials. - : WILEY-V C H VERLAG GMBH. - 0935-9648 .- 1521-4095. ; 34:32
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Tidskriftsartikel (refereegranskat)abstract
- Organic solar cells (OSCs) have experienced rapid progress with the innovation of near-infrared (NIR)-absorbing small-molecular acceptors (SMAs), while the unique electronic properties of the SMAs raise new challenges in relation to cathode engineering for effective electron collection. To address this issue, two fluorinated perylene-diimides (PDIs), PDINN-F and PDINN-2F, are synthesized by a simple fluorination method, for application as cathode interlayer (CIL) materials. The two bay-fluorinated PDI-based CILs possess a lower lowest unoccupied molecular orbital (LUMO) energy level of approximate to-4.0 eV, which improves the energy level alignment at the NIR-SMAs (such as BTP-eC9)/CIL for a favorable electron extraction efficiency. The monofluorinated PDINN-F shows higher electron mobility and better improved interfacial compatibility. The PDINN-F-based OSCs with PM6:BTP-eC9 as active layer exhibit an enhanced fill factor and larger short-circuit current density, leading to a high power conversion efficiency (PCE) exceeding 18%. The devices with PDINN-F CIL retain more than 80% of their initial PCE after operating at the maximum power point under continuous illumination for 750 h. This work prescribes a facile, cost-effective, and scalable method for the preparation of stable, high-performance fluorinated CILs, and instilling promise for the NIR-SMAs-based OSCs moving forward.
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| 39. |
- Ye, Yin, et al.
(författare)
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Efficient and durable uranium extraction from uranium mine tailings seepage water via a photoelectrochemical method
- 2021
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Ingår i: iScience. - : Elsevier BV. - 2589-0042. ; 24:11
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Tidskriftsartikel (refereegranskat)abstract
- Current photocatalytic uranium (U) extraction methods have intrinsic obstacles, such as the recombination of charge carriers, and the deactivation of catalysts by extracted U. Here we show that, by applying a bias potential on the photocatalyst, the photoelectrochemical (PEC) method can address these limitations. We demonstrate that, owing to efficient spatial charge-carriers separation driven by the applied bias, the PEC method enables efficient and durable U extraction. The effects of multiple operation conditions are investigated. The U extraction proceeds via single-step one-electron reduction, resulting in the formation of pentavalent U, which can facilitate future studies on this often-overlooked U species. In real seepage water the PEC method achieves an extraction capacity of 0.67 gU m(-3).h(-1) without deactivation for 156 h continuous operation, which is 17 times faster than the photocatalytic method. This work provides an alternative tool for U resource recovery and facilitates future studies on U(V) chemistry.
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| 40. |
- Ye, Yin, et al.
(författare)
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Electrochemical removal and recovery of uranium: Effects of operation conditions, mechanisms, and implications
- 2022
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Ingår i: Journal of Hazardous Materials. - : Elsevier BV. - 1873-3336 .- 0304-3894. ; 432
-
Tidskriftsartikel (refereegranskat)abstract
- Removing and recovering uranium (U) from U-mining wastewater would be appealing, which simultaneously reduces the adverse environmental impact of U mining activities and mitigates the depletion of conventional U resources. In this study, we demonstrate the application of a constant-voltage electrochemical (CVE) method for the removal and recovery of U from U-mining wastewater, in an ambient atmosphere. The effects of operation conditions were elucidated in synthetic U-bearing water experiments, and the cell voltage and the ionic strength were found to play important roles in both the U extraction kinetics and the operation cost. The mechanistic studies show that, in synthetic U-bearing water, the CVE U extraction proceeds exclusively via a single-step one-electron reduction mechanism, where pentavalent U is the end product. In real U-mining wastewater, the interference of water matrices led to the disproportionation of the pentavalent U, resulting in the formation of tetravalent and hexavalent U in the extraction products. The U extraction efficacy of the CVE method was evaluated in real U-mining wastewater, and results show that the CVE U extraction method can be efficient with operation costs ranging from $0.55/kgU ~ $64.65/kgU, with varying cell voltages from 1.0 V to 4.0 V, implying its feasibility from the economic perspective.
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| 41. |
- Zhang, Yu, et al.
(författare)
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Comparative phylogenomics and phylotranscriptomics provide insights into the genetic complexity of nitrogen-fixing root-nodule symbiosis
- 2024
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Ingår i: Plant communications. - 2590-3462. ; 5:1
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Tidskriftsartikel (refereegranskat)abstract
- Plant root-nodule symbiosis (RNS) with mutualistic nitrogen-fixing bacteria is restricted to a single clade of angiosperms, the Nitrogen-Fixing Nodulation Clade (NFNC), and is best understood in the legume family. Nodulating species share many commonalities, explained either by divergence from a common ancestor over 100 million years ago or by convergence following independent origins over that same time period. Regardless, comparative analyses of diverse nodulation syndromes can provide insights into constraints on nodulation-what must be acquired or cannot be lost for a functional symbiosis-and the latitude for variation in the symbiosis. However, much remains to be learned about nodulation, especially outside of legumes. Here, we employed a large-scale phylogenomic analysis across 88 species, complemented by 151 RNA-seq libraries, to elucidate the evolution of RNS. Our phylogenomic analyses further emphasize the uniqueness of the transcription factor NIN as a master regulator of nodulation and identify key mutations that affect its function across the NFNC. Comparative transcriptomic assessment revealed nodulespecific upregulated genes across diverse nodulating plants, while also identifying nodule-specific and nitrogen-response genes. Approximately 70% of symbiosis-related genes are highly conserved in the four representative species, whereas defense-related and host-range restriction genes tend to be lineage specific. Our study also identified over 900 000 conserved non-coding elements (CNEs), over 300 000 of which are unique to sampled NFNC species. NFNC-specific CNEs are enriched with the active H3K9ac mark and are correlated with accessible chromatin regions, thus representing a pool of candidate regulatory elements for genes involved in RNS. Collectively, our results provide novel insights into the evolution of nodulation and lay a foundation for engineering of RNS traits in agriculturally important crops.
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