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1.
Inorg Chem ; 63(1): 833-841, 2024 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-38115192

RESUMO

Luminescent bulk crystals exhibit fewer grain boundaries and defects compared with conventional microsized powdery ones. Herein, targeting Mn4+-activated fluoride crystals with a sharp line-type red luminescence spectrum, we propose a new cooling-induced crystallization method to grow the fluoride crystals. By this new method, we successfully grew millimeter-sized K2MnF6:Si4+, NH4+ crystals, featuring an AEmax (absorption efficiency) of 93.5% and an EQEmax (external quantum efficiency) of 68.9%, which are among the best values for Mn4+-activated fluoride red phosphors. The influence of doping Si4+ and/or NH4+ in K2MnF6 on the local coordination structure and luminescence properties was studied. The anomalous thermal quenching behaviors were discussed, the luminescence decay from the excited state was compared, and the origin for the high quantum efficiencies was analyzed.

2.
Phys Chem Chem Phys ; 25(4): 3182-3189, 2023 Jan 27.
Artigo em Inglês | MEDLINE | ID: mdl-36622128

RESUMO

The structure and electronic and spintronic properties of two-dimensional (2D) ternary compounds ABC (A = Sb, Bi; B = Se, Te; C = Br; I) monolayers are investigated using the first-principles method. The ABC monolayers possess typical Janus structures with a considerable potential gradient normal to the surface, inducing intrinsic Rashba spin splitting (RSS) at the conduction band minimum near the Γ point. Among them, the splitting strength of the BiSeI monolayer is the largest and its Rashba coefficient can reach 1.84 eV Å. The projected energy band of the BiSeI monolayer suggests that the RSS state is mainly rooted in the Bi-pz orbital. The RSS strength can be modulated by applying the in-plane strain. The tensile strain can improve the RSS strength, which is ascribed to the increase of the potential gradient normal to the surface. These results indicate that these 2D ternary compounds have great potential for application in tunable spintronic devices.

3.
Phys Chem Chem Phys ; 24(46): 28295-28305, 2022 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-36382798

RESUMO

Janus α-STe2 and α-SeTe2 monolayers are investigated systematically using first-principles calculations combined with semiclassical Boltzmann transport theory. Janus α-STe2 and α-SeTe2 monolayers are indirect semiconductors with band gaps of 1.20 and 0.96 eV, respectively. It is found that they possess ultrahigh figure of merit (ZT) values of 3.9 and 4.4, respectively, at 500 K, much higher than that of the pristine α-Te monolayer (2.8). The higher ZT values originating from Janus structures reduce lattice thermal conductivities remarkably compared with the pristine α-Te monolayer. The much higher phonon anharmonicity in Janus monolayers leads to significantly lower lattice thermal conductivity. It is also found that electronic thermal conductivity can play an important role in thermoelectric efficiency of materials with quite low lattice thermal conductivity. This work suggests the potential applications of Janus α-STe2 and α-SeTe2 monolayers as thermoelectric materials and highlights that using a Janus structure is an effective way to enhance thermoelectric performance.

4.
J Oral Rehabil ; 49(2): 265-271, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34902183

RESUMO

BACKGROUND: Chewing side preference (CSP) could cause structural and morphological changes of temporomandibular joint (TMJ) and has been suggested as one aetiology of temporomandibular disorders (TMDs), but the condylar position in TMD patients with CSP is unknown. OBJECTIVE: To compare the condylar position in the TMD patients with and without CSP. METHODS: Ninety TMD patients with unilateral symptom (69 with CSP and 21 without CSP) and 20 asymptomatic participants received cone-beam computed tomography. The condylar position was determined based on the measurements of sagittal joint spaces. Intergroup and intra-group comparisons of the condylar position were performed. RESULTS: The condyles in asymptomatic participants located nearly randomly in anterior, centric and posterior positions. Patients without CSP had significantly more posterior condyles than asymptomatic participants (57.1% vs 30.0%, p < 0.05). In patients with CSP, 50.7% of the condyles on the preferred chewing side and 42.0% on the unpreferred side located posteriorly, reaching no significant level compared with the asymptomatic participants and patients without CSP (p > 0.05). The symptomatic joints and asymptomatic joints in patients with CSP and without CSP showed no significant differences in condylar position. While patients without CSP had significantly more posterior condyles in symptomatic joints than asymptomatic participants (p < 0.05), patients with CSP showed a trend towards more posterior condyles in symptomatic joints compared with the asymptomatic participants (53.6% vs 30.0%, p = 0.054). CONCLUSION: Condylar position is not a strong indicator to differentiate CSP-related TMDs from non-CSP-related TMDs. Posterior condyle could not be viewed as one indicator of TMD.


Assuntos
Mastigação , Transtornos da Articulação Temporomandibular , Tomografia Computadorizada de Feixe Cônico , Humanos , Côndilo Mandibular/diagnóstico por imagem , Articulação Temporomandibular/diagnóstico por imagem , Transtornos da Articulação Temporomandibular/diagnóstico por imagem
5.
Inorg Chem ; 60(17): 13212-13221, 2021 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-34379393

RESUMO

Due to the low solubility of BaF2, the BaTiF6:Mn4+ phosphor for whitelight-emitting diodes application has been generally synthesized by the hydrothermal route, during which process the valence of the manganese dopant is difficult to be controlled as tetravalent. In this paper, a new synthesis method that proceeded at room temperature was reported. This method uses BaTiOF4 as the precursor and allows for the control of the phase transformation rate from BaTiOF4 to BaTiF6 in the K2MnF6/HF acid solution. Benefitting from that, we successfully prepared red-emitting BaTiF6:Mn4+ elongated crystals with a single-crystal nature up to a record-breaking length of 200-300 µm. The effects of the crystallinity of the BaTiOF4 precursor on its phase transformation rate into BaTiF6 and on the optimal Mn4+ doping concentration were studied. The BaTiF6:Mn4+ single-crystal phosphor exhibits relatively excellent hydrolysis-resistant behavior after being immersed in water for 3 h, at which condition the commercial K2SiF6:Mn4+ has become brown. This study may inspire the room-temperature preparation of other hydrolysis-resistant alkali earth fluorotitanate or fluorosilicate phosphors with stable tetravalent manganese doping.

6.
BMC Oral Health ; 21(1): 396, 2021 08 13.
Artigo em Inglês | MEDLINE | ID: mdl-34389008

RESUMO

BACKGROUND: Chewing side preference (CSP) has been proposed as one etiology of temporomandibular disorders (TMDs) as it can induce the structural changes of the temporomandibular joint. But its association with the inclination of the articular eminence (IAE) is unknown. This study aimed to compare IAE between patients with CSP and without CSP. METHODS: Cone-beam computed tomography images of 90 patients with TMD (mean age of 45.6 years, 69 with CSP, 21 without CSP) and 20 participants without TMD and CSP (mean age of 41.3 years) were measured to compare IAE and depth of the glenoid fossa (DGF) RESULTS: IAE and DGF showed a positive correlation among all the participants. Compared with the participants without TMD and CSP, the TMD patients without CSP presented a similar IAE but with a significantly higher value of DGF (p < 0.05); in contrast, the TMD patients with CSP presented a significantly greater IAE and DGF (p < 0.05). No bilateral differences in IAE and DGF were observed in all the participants. Except the male patients with CSP had a deeper fossa than did the female, no differences in IAE and DGF according to gender were observed. CONCLUSIONS: TMD patients with CSP seem to have a deep glenoid fossa with steep eminence which might be considered one characteristic imaging feature.


Assuntos
Procedimentos de Cirurgia Plástica , Transtornos da Articulação Temporomandibular , Adulto , Tomografia Computadorizada de Feixe Cônico , Feminino , Humanos , Masculino , Mastigação , Pessoa de Meia-Idade , Articulação Temporomandibular/diagnóstico por imagem , Transtornos da Articulação Temporomandibular/diagnóstico por imagem
7.
Angew Chem Int Ed Engl ; 60(9): 4872-4878, 2021 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-33197111

RESUMO

Hot electrons activate reactants and reduce the activation energy barrier (Ea ) of a reaction through electron donation. However, a comprehensive understanding of the intrinsic driving force of this electron-donating effect is lacking, let alone the precise manipulation of electron donation processes. Herein, the essential and promotional role of hot electron energy on the electron-donating effect was elucidated using molecular oxygen activation (MOA) as a model reaction. Through providing an available electron source to the conventional photo-thermal conversion system, the high energy carried by hot electrons was liberated and greatly enhanced the electron donation towards the LUMO (π*) orbit of O2 . The energy was also transferred to O2 and elevated the potential energy surface (PES) of MOA, which was reflected by the enhanced formation of superoxide oxygen anions. As predicted, the Ea of MOA decreased by 45.1 % and exhibited a substantial light dependence, demonstrating that MOA became energy-efficient due to improved exploitation and conversion of photon energies.

8.
J Am Chem Soc ; 142(9): 4136-4140, 2020 Mar 04.
Artigo em Inglês | MEDLINE | ID: mdl-32081005

RESUMO

Hydrogen doping of metal oxide semiconductors is promising for manipulation of their properties toward various applications. Yet it is quite challenging because it requires harsh reaction conditions and expensive metal catalysts. Meanwhile, acids as a cheap source of protons have long been unappreciated. Here, we develop a sophisticated acid-metal treatment for tunable hydrogenation of metal oxides at ambient conditions. Using first-principles simulations, we first show that, with proper work function difference between the metal and metal oxide, H-diffusion into negatively charged metal oxide can be well controlled, resulting in tunable H-doping of metal oxides with quasi-metal characteristics. This has been verified by proof-of-concept experiments that achieved the controllable hydrogenation of WO3 using Cu and hydrochloric acid at ambient conditions. Further, H-doping of other metal oxides (TiO2/Nb2O5/MoO3) has been achieved by metal-acid treatment and induced a change in properties. Our work provides a promising way to tailor metal oxides via tunable H-doping.

9.
Inorg Chem ; 59(24): 18374-18383, 2020 Dec 21.
Artigo em Inglês | MEDLINE | ID: mdl-33244973

RESUMO

A single-crystalline defect-less phosphor is desired for efficient luminescence of the therein doped optical activators. In this paper, microsized MgAl2O4:Mn4+ single-crystal phosphors with bright red luminescence were grown in molten LiCl salt at 950 °C, for application in blue LED pumped white lighting. By comparing the phosphor formation from various Mg2+- and Al3+-bearing sources, both the template-formation and the dissolution-diffusion processes were evidenced to account for the formation of the microsized MgAl2O4:Mn4+ crystallites. Using nano γ-Al2O3 as the Al3+-bearing precursor, the uniform MgAl2O4:Mn4+ microcrystallites with a {111} planes-exposed tetragonal bipyramid morphology were obtained. The photoluminescence property was studied at various temperatures, and Mg ↔ Al anti-site disorder induced luminescence broadening was discussed. The Mn4+ 2Eg → 4A2g transition in MgAl2O4 shows a quite short luminescence wavelength peaking at 651 nm and ultrabroadband emission extending to 850 nm. The luminescence is relatively robust against thermal effect with relatively high thermal quenching temperature of 400 K and activation energy of 0.23 eV. Employing the red-emitting MgAl2O4:Mn4+ crystallites, blue LED pumped white lighting prototypes were fabricated which simulate the solar-like spectrum and show neutral to warm white.

10.
Phys Chem Chem Phys ; 22(38): 21961-21967, 2020 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-32974632

RESUMO

Mexican-hat-like band dispersion is extremely critical to the realization of hole-doping-induced magnetism in monolayer metal monochalcogenides. However, it is absent from transition-metal dichalcogenides (TMDCs), i.e., WSe2. Herein, using first-principles calculations, we show that Mexican-hat-like band dispersion can be achieved by applying interlayer strain (ε) in the WSe2/SnS2 van der Waals (vdW) heterostructure when ε exceeds 15%. This is because in the strain-induced distorted trigonal prismatic crystal field, at the valence band edge, the W_dz2 orbitals shift upward around the Γ point, while the double-degenerate W_dxy/dx2-y2 orbitals shift downward at the K point, resulting in Mexican-hat-like band dispersion near the Γ point when the energy level of the Γ point surpasses that of the K point. On account of the appearance of the Mexican-hat-like band edge (MHBE), hole-doping in the strained WSe2/SnS2 heterostructure induces magnetization readily from the nonmagnetized phase. Our findings may provide a new strategy for the realization of magnetized TMDC-based vdW heterostructures.

11.
Angew Chem Int Ed Engl ; 58(39): 13711-13716, 2019 Sep 23.
Artigo em Inglês | MEDLINE | ID: mdl-31332923

RESUMO

Charge doping is an effective way to induce the metal-insulator transition (MIT) in correlated materials for many important utilizations, which is however practically limited by problem of low stability. An electron-proton co-doping mechanism is used to achieve pronounced phase modulation of monoclinic vanadium dioxide (VO2 ) at room temperature. Using l-ascorbic acid (AA) solution to treat VO2 , the ionized AA- species donate electrons to the adsorbed VO2 surface. Charges then electrostatically attract surrounding protons to penetrate, and eventually results in stable hydrogen-doped metallic VO2 . The variations of electronic structures, especially the electron occupancy of V 3d/O 2p hybrid orbitals, were examined by synchrotron characterizations and first-principle theoretical simulations. The adsorbed molecules protect hydrogen dopants from escaping out of lattice and thereby stabilize the metallic phase for VO2 .

12.
J Phys Chem A ; 121(22): 4225-4232, 2017 Jun 08.
Artigo em Inglês | MEDLINE | ID: mdl-28528553

RESUMO

Room-temperature phosphorescence (RTP) from purely organic systems is of practical importance in biological imaging, oxygen sensing and displaying technologies. The key step to obtaining RTP from organic molecules is efficient intersystem crossing (ISC), which is usually low compared to inorganic materials. Here we show that protonation of a dye molecule, a thioflavin derivative, in strongly polar polyurethane can be used to effectively harness RTP. Prior to protonation, the predominant transition is π-π* for the polymer, which has nearly undetectable RTP due to the large singlet-triplet energy splitting (0.87 eV); when Brønsted acids are gradually added to the system, increasingly strong RTP is observed due to the presence of a new intramolecular charge-transfer state (ICT). The ICT state serves to lower the singlet-triplet energy gap (0.46 eV). The smaller gap results in more efficient ISC and thus strong RTP under deoxygenated conditions. The thioflavin-polyurethane system can be tuned via proton concentration and counterions and opens new doors for RTP-based polymeric sensors and stimuli-responsive materials.

13.
Nat Commun ; 15(1): 5814, 2024 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-38987527

RESUMO

For first-order phase transitions, the second derivatives of Gibbs free energy (specific heat and compressibility) diverge at the transition point, resulting in an effect known as super-elasticity along the pressure axis, or super-thermicity along the temperature axis. Here we report a chemical analogy of these singularity effects along the atomic doping axis, where the second derivative of Gibbs free energy (chemical susceptibility) diverges at the transition point, leading to an anomalously high energy barrier for dopant diffusion in co-existing phases, an effect we coin as super-susceptibility. The effect is realized in hydrogen diffusion in vanadium dioxide (VO2) with a metal-insulator transition (MIT). We show that hydrogen faces three times higher energy barrier and over one order of magnitude lower diffusivity when it diffuses across a metal-insulator domain wall in VO2. The additional energy barrier is attributed to a volumetric energy penalty that the diffusers need to pay for the reduction of latent heat. The super-susceptibility and resultant retarded atomic diffusion are expected to exist universally in all phase transformations where the transformation temperature is coupled to chemical composition, and inspires new ways to engineer dopant diffusion in phase-coexisting material systems.

14.
J Huazhong Univ Sci Technolog Med Sci ; 33(2): 303-308, 2013 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-23592148

RESUMO

The purpose of this study was to investigate the cortical bone thickness of the inter-dental area of both jaws for orthodontic miniscrew placement. The cone-beam computerized tomography images of 32 non-orthodontic adults with normal occlusion were taken to measure the cortical bone thickness in both jaws. One-way analysis of variance (ANOVA) was used to analyze the differences in cortical bone thickness. Buccal cortical bone in the mandible was thicker than that in the maxilla. In the maxilla, cortical bone thickness was thicker in the buccal side than in the palatal side. Buccal cortical bone thickness in the mandible was thickest at the site distal to the first molar, and in the maxilla it was thickest at the site mesial to the first molar, while in the palatal side of maxilla it was thickest at the site mesial to the second premolar. The changing pattern of cortical bone thickness varies at different sites. In the buccal side of maxilla, the thinnest cortical bone thickness was found to be at 4 mm level from the alveolar crest, while the thickest was at 10 mm level (except for the site mesial to the first premolar). The buccal cortical bone thickness at the sites mesial or distal to the first molar in the mandible and palatal cortical bone thickness of maxilla tended to increase with increasing distance from the alveolar bone.


Assuntos
Parafusos Ósseos , Tomografia Computadorizada de Feixe Cônico/métodos , Implantação Dentária Endo-Óssea Endodôntica/instrumentação , Mandíbula/diagnóstico por imagem , Mandíbula/cirurgia , Maxila/diagnóstico por imagem , Maxila/cirurgia , Adulto , Implantação Dentária Endo-Óssea Endodôntica/métodos , Feminino , Humanos , Masculino , Radiografia Dentária/métodos , Reprodutibilidade dos Testes , Sensibilidade e Especificidade , Cirurgia Assistida por Computador/métodos , Adulto Jovem
15.
Adv Sci (Weinh) ; 10(4): e2205347, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36479607

RESUMO

Vacancy engineering is deemed as one of the powerful protocols to tune the catalytic activity of electrocatalysts. Herein, Se-vacancy with charge polarization is created in the NiSe2 structure (NiSe2 -VSe ) via a sequential phase conversion strategy. By a combined analysis of the Rietveld method, transient photovoltage spectra (TPV), in situ Raman and density functional theory (DFT) calculation, it is unequivocally discovered that the presence of charge-polarized Se-vacancy is beneficial for stabilizing the structure, decreasing the electron transfer kinetics, as well as optimizing the free adsorption energy of reaction intermediate during two-electron oxygen reduction reaction (2e- ORR). Benefiting from these merits, the as-prepared NiSe2 -VSe delivered the highest selectivity of 96% toward H2 O2 in alkaline media, together with a selectivity higher than 90% over the wide potential range from 0.25 to 0.55 V, ranking it in the top level among the previously reported transition metal-based electrocatalysts. Most notably, it also displayed admirable stability with only a slight selectivity decay after 5000 cycles of accelerated degradation test (ADT).

16.
Adv Mater ; 35(11): e2208337, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-36528302

RESUMO

A hydrogen processing strategy is developed to enable bulk LaNi5 to attain high activity and long-term stability toward the electrocatalytic oxygen evolution reaction (OER). By a combination of in situ Raman and quasi in situ X-ray absorption (XAS) spectra, secondary-electron-excited scanning transmission electron microscopy (STEM) patterns as well as the Rietveld method and density functional theory (DFT) calculations, it is discovered that hydrogen-induced lattice distortion, grain refinement, and particle cracks dictate the effective reconstruction of the LaNi5 surface into a porous hetero-nanoarchitecture composed of uniformly confined active γ-NiOOH nanocrystals by La(OH)3 layer in the alkaline OER process. This significantly optimizes the charge transfer, structural integrity, active-site exposure, and adsorption energy toward the reaction intermediates. Benefiting from these merits, the overpotential (322 mV) at 100 mA cm-2 for the hydrogen-processed OER catalyst deposited on nickel foam is reduced by 104 mV as compared to the original phase. Notably, it exhibits remarkable stability for 10 days at an industrial-grade current density of more than 560 mA cm-2 in alkaline media.

17.
Nanomicro Lett ; 15(1): 186, 2023 Jul 29.
Artigo em Inglês | MEDLINE | ID: mdl-37515724

RESUMO

Efficient and durable oxygen evolution reaction (OER) requires the electrocatalyst to bear abundant active sites, optimized electronic structure as well as robust component and mechanical stability. Herein, a bimetallic lanthanum-nickel oxysulfide with rich oxygen vacancies based on the La2O2S prototype is fabricated as a binder-free precatalyst for alkaline OER. The combination of advanced in situ and ex situ characterizations with theoretical calculation uncovers the synergistic effect among La, Ni, O, and S species during OER, which assures the adsorption and stabilization of the oxyanion [Formula: see text] onto the surface of the deeply reconstructed porous heterostructure composed of confining NiOOH nanodomains by La(OH)3 barrier. Such coupling, confinement, porosity and immobilization enable notable improvement in active site accessibility, phase stability, mass diffusion capability and the intrinsic Gibbs free energy of oxygen-containing intermediates. The optimized electrocatalyst delivers exceptional alkaline OER activity and durability, outperforming most of the Ni-based benchmark OER electrocatalysts.

18.
Nanomaterials (Basel) ; 13(1)2022 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-36616052

RESUMO

In this paper, mesoporous CuO with a novel architecture was synthesized through a conventional hydrothermal approach followed by a facile sintering procedure. HR-TEM analysis found that mesoporous CuO with an interconnected pore structure has exposed high-energy crystal planes of (002) and (200). Theoretical calculations indicated that the high-energy crystal planes have superior adsorption capacity for H+ ions, which is critical for the excellent adsorption and remarkable photocatalytic activity of the anionic dye. The adsorption capacity of CuO to methyl orange (MO) at 0.4 g/L was approximately 30% under adsorption equilibrium conditions. We propose a state-changing mechanism to analyze the synergy and mutual restraint relation among the catalyst CuO, H+ ions, dye and H2O2. According to this mechanism, the degradation rate of MO can be elevated 3.5 times only by regulating the MO ratio in three states.

19.
Small Methods ; 6(12): e2200931, 2022 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-36287026

RESUMO

The utilization of clean hydrogen energy is becoming more feasible for the sustainable development of this society. Considering the safety issues in the hydrogen production, storage, and utilization, a sensitive hydrogen sensor for reliable detection is essential and highly important. Though various gas sensor devices are developed based on tin oxide, tungsten trioxide, or other oxides, the relatively high working temperature, unsatisfactory response time, and detection limitation still affect the extensive applications. In the current study, an amorphous tungsten trioxide (a-WO3 ) layer is deposited on a phase-change vanadium dioxide film to fabricate a phase transition controlled Pd/a-WO3 /VO2 hydrogen sensor for hydrogen detection. Results show that both the response time and sensitivity of the hydrogen sensor are improved greatly if increasing the working temperature over the transition temperature of VO2 . Theoretical calculations also reveal that the charge transfer at VO2 /a-WO3 interface becomes more pronounced once the VO2 layer transforms to the metal state, which will affect the migration barrier of H atoms in a-WO3 layer and thus improve the sensor performance. The current study not only realizes a hydrogen sensor with ultrahigh performance based on VO2 layer, but also provides some clues for designing other gas sensors with phase-change material.

20.
RSC Adv ; 11(39): 24366-24373, 2021 Jul 06.
Artigo em Inglês | MEDLINE | ID: mdl-35479044

RESUMO

Tuning the interlayer twist angle provides a new degree of freedom to exploit the potentially excellent properties of two dimensional layered materials. Here we investigate the structural and electronic properties of twisted bilayer SiC under a series of twist angles using first principle calculations. The interplay of interlayer van der Waals interactions and intralayer strain induces dramatic in-plane and out-of-plane displacements. The expansion or contraction of specific stacking domains can be interpreted as the result of the energy minimization rule. By means of order parameter analysis, the triangular or hexagonal strain soliton networks are found to separate adjacent stacking domains. The unique overlapped zigzag atom lines in strain solitons provide a unique characteristic for experimental imaging. The top valence band and bottom conduction band evolve into flat bands with the smallest band width of 4 meV, indicating a potential Mott-insulator phase. The moiré-potential-modulated localization pattern of states in the flat band, which is dependent sensitively on the structure relaxation, controls the flat band width. The moiré-pattern-induced structural and electronic properties of twisted bilayer SiC are promising for application in nanoscale electronic and optical devices.

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