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1.
Small ; : e2003357, 2020 Aug 02.
Artigo em Inglês | MEDLINE | ID: mdl-32743967

RESUMO

Monolayer transition metal dichalcogenides are 2D materials with many potential applications. Chemical vapor deposition (CVD) is a promising method to synthesize these materials. However, CVD-grown materials generally have poorer quality than mechanically exfoliated ones and contain more defects due to the difficulties in controlling precursors' distribution and concentration during growth where solid precursors are used. Here, thiol is proposed to be used as a liquid precursor for CVD growth of high quality and uniform 2D MoS2 . Atomic-resolved structure characterizations indicate that the concentration of sulfur vacancies in the MoS2 grown from thiol is the lowest among all reported CVD samples. Low temperature spectroscopic characterization further reveals the ultrahigh optical quality of the grown MoS2 . Density functional theory simulations indicate that thiol molecules could interact with sulfur vacancies in MoS2 and repair these defects during the growth of MoS2 , resulting in high-quality MoS2 . This work provides a facile and controllable method for the growth of high-quality 2D materials with ultralow sulfur vacancies and high optical quality, which will benefit their optoelectronic applications.

2.
Nat Commun ; 11(1): 3399, 2020 Jul 07.
Artigo em Inglês | MEDLINE | ID: mdl-32636385

RESUMO

As a key building block of biological cortex, neurons are powerful information processing units and can achieve highly complex nonlinear computations even in individual cells. Hardware implementation of artificial neurons with similar capability is of great significance for the construction of intelligent, neuromorphic systems. Here, we demonstrate an artificial neuron based on NbOx volatile memristor that not only realizes traditional all-or-nothing, threshold-driven spiking and spatiotemporal integration, but also enables dynamic logic including XOR function that is not linearly separable and multiplicative gain modulation among different dendritic inputs, therefore surpassing neuronal functions described by a simple point neuron model. A monolithically integrated 4 × 4 fully memristive neural network consisting of volatile NbOx memristor based neurons and nonvolatile TaOx memristor based synapses in a single crossbar array is experimentally demonstrated, showing capability in pattern recognition through online learning using a simplified δ-rule and coincidence detection, which paves the way for bio-inspired intelligent systems.

3.
J Periodontal Res ; 2020 Jun 25.
Artigo em Inglês | MEDLINE | ID: mdl-32583879

RESUMO

Periodontal disease (PD), as a chronic bacterial infection, might cause cardiovascular and some other systemic diseases, with recent studies reporting that it exhibits some connection with lung cancer. While studies have shown that poor oral health might increase the risk of lung cancer, the veracity of these reports is questionable. Therefore, this meta-analysis was undertaken to investigate the association between PD and the risk of lung cancer. A search was run in PubMed, EMBASE, MEDLINE, CENTRAL, and ClinicalTrials.gov databases up to January 1, 2020. Cohort and case-control studies investigating the correlation between PD and lung cancer were included. Eligibility assessment and data extraction were conducted independently, and a meta-analysis was performed to synthesize the data. The association between PD, edentulism, and lung cancer was measured by the adjusted hazard ratios (HRs) or odds ratios (ORs) and their 95% confidence intervals (CIs) provided in articles. We employed appropriate effect model in terms of I2 (a fixed-effect model for PD and a random-effect model for edentulism) to obtain summary effect estimates. Statistical heterogeneity was investigated by chi-square test and I2 statistics. Newcastle-Ottawa Scale (NOS) was used to assess the quality of their method. Six cohort studies (eight references) and two case-control studies, assessed as high-quality, involving 167 256 participants, were included in the review. The summary estimates based on adjusted data showed an association between PD and a significant risk of lung cancer both in cohort studies (HR = 1.40, 95% CI = 1.25-1.58; I2  = 8.7%) and case-control studies (OR = 1.51, 95% CI = 1.16-1.98; I2  = 36.5%). Similar features were found in the sensitivity analysis and subgroups for six cohort studies, of male only (HR = 1.36, 95% CI = 1.15-2.60), setting the lung cancer incidence as endpoint (HR = 1.39, 95% CI = 1.24-1.57; I2  = 23.9%), and adjusting alcohol for multifactorial HR (HR = 1.38, 95% CI = 1.21-1.57; I2  = 39.9%). The summary HR for edentulism was 1.93 (95% CI = 1.05-3.57; I2  = 55.3%). No obvious publication bias was detected. This systematic review and meta-analysis demonstrated a significant association between PD and the incidence of lung cancer. Further observational studies are required by using standardized measurements to assess the periodontal status and by eliminating confounding factors, such as alcohol and diabetes, to verify such a relationship.

4.
Adv Mater ; : e2001167, 2020 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-32567078

RESUMO

Lack of effective strategies to regulate the internal activity of MoS2 limits its practical application for hydrogen evolution reactions (HERs). Doping of heteroatoms without forming aggregation or an edge enrichment is still challenging, and its effect on the HER needs to be further explored. Herein, a two-step method is developed to obtain multi-metal-doped H-MoS2 , which includes intercalation of the layered MoO3 precursor with a following sulfurization. Benefiting from the capability of the intercalation method to uniformly and simultaneously introduce different elements into the van der Waals gap, this method is universal to obtain multi-heteroatoms co-doped MoS2 without forming clusters, phase separation, and an edge enrichment. It is demonstrated that the doping of adjacent cobalt and palladium monomers on MoS2 greatly enhances the HER catalytic activity. The overpotential at 10 mA cm-2 and Tafel slope of Co and Pd co-doped MoS2 is found to be 49.3 mV and 43.2 mV dec-1 , respectively, representing a superior acidic HER catalytic activity. This intercalation-assisted method also provides a new and general strategy to synthesize uniformly doped transition metal dichalcogenides for various applications.

5.
ACS Nano ; 2020 Apr 13.
Artigo em Inglês | MEDLINE | ID: mdl-32267670

RESUMO

Two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs) have emerged as attractive platforms in next-generation nanoelectronics and optoelectronics for reducing device sizes down to a 10 nm scale. To achieve this, the controlled synthesis of wafer-scale single-crystal TMDs with high crystallinity has been a continuous pursuit. However, previous efforts to epitaxially grow TMD films on insulating substrates (e.g., mica and sapphire) failed to eliminate the evolution of antiparallel domains and twin boundaries, leading to the formation of polycrystalline films. Herein, we report the epitaxial growth of wafer-scale single-crystal MoS2 monolayers on vicinal Au(111) thin films, as obtained by melting and resolidifying commercial Au foils. The unidirectional alignment and seamless stitching of the MoS2 domains were comprehensively demonstrated using atomic- to centimeter-scale characterization techniques. By utilizing onsite scanning tunneling microscope characterizations combined with first-principles calculations, it was revealed that the nucleation of MoS2 monolayer is dominantly guided by the steps on Au(111), which leads to highly oriented growth of MoS2 along the ⟨110⟩ step edges. This work, thereby, makes a significant step toward the practical applications of MoS2 monolayers and the large-scale integration of 2D electronics.

6.
J Phys Chem Lett ; : 3152-3158, 2020 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-32239941

RESUMO

Two-dimensional van der Waals (vdW) magnetic materials are well-recognized milestones toward nanostructured spintronics. An interesting example is CrI3; its magnetic states can be modulated electrically, allowing spintronics applications that are highly compatible with electronics technologies. Here, we report the electric field alone induces the interlayer antiferromagnetic-to-ferromagnetic (AFM-to-FM) phase transition in CrI3 bilayers with critical field as low as 0.12 V/Å. The AFM-FM energy difference ΔE increases with electric field and is closely related to the field-induced on-site energy difference defined as the splitting between the electronic states of the two vdW layers. Our tight-binding model fits closely with ΔE as a function of electric field and gives a consistent estimation for orbital hopping, exchange splitting, and crystal field splitting. Furthermore, a CrI3-based spin field-effect device is suggested with the spin current switched on and off solely by the electric field. These findings not only reveal the physics underlying the transition but also provide guidelines for future discovery and design.

7.
Sci Adv ; 6(7): eaay4092, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-32110729

RESUMO

Intercalated transition metal dichalcogenides (TMDs) have attracted substantial interest due to their exciting electronic properties. Here, we report a unique approach where copper (Cu) atoms from bulk Cu solid intercalate spontaneously into van der Waals (vdW) gaps of group IV and V layered TMDs at room temperature and atmospheric pressure. This distinctive phenomenon is used to develop a strategy to synthesize Cu species-intercalated layered TMD compounds. A series of Cu-intercalated 2H-NbS2 compounds were obtained with homogeneous distribution of Cu intercalates in the form of monovalent Cu (I), occupying the tetrahedral sites coordinated by S atoms within the interlayer space of NbS2. The Fermi level of NbS2 shifts up because of the intercalation of Cu, resulting in the improvement of electrical conductivity in the z-direction. On the other hand, intercalation of Cu into vdW gaps of NbS2 systematically suppresses the superconducting transition temperature (T c) and superconducting volume fraction.

8.
J Phys Chem Lett ; : 1644-1649, 2020 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-32046495

RESUMO

The transformation of 2H-MoS2 from semiconducting 2H to metallic 1T phases is critical for its electrochemical and device applications, where the formation and dynamics of electronic heterostructures play a key role. Using first-principles calculations, we explore detailed atomic structures and migration processes of such interfaces. While armchair interfacial bonding is severely weakened by the distortion in 1T phase, stable structures form for either Mo- or S-orientated zigzag interfaces with low contact resistance. Different zigzag interfaces have distinct local bonding, which renders interface migration behaviors strongly anisotropic. For Mo-oriented interfaces, both a low formation energy and the migration barrier of the kinks make them prone to fast migration. In contrast, the S-oriented interfaces are more immobile due to the high formation energies of kinks and thus dominate the physical properties of the whole heterostructures. Our findings not only explain various experimental observations but also provide insights into phase transition behaviors in 2D MoS2.

9.
Nature ; 577(7791): 492-496, 2020 01.
Artigo em Inglês | MEDLINE | ID: mdl-31969724

RESUMO

Although two-dimensional (2D) atomic layers, such as transition-metal chalcogenides, have been widely synthesized using techniques such as exfoliation1-3 and vapour-phase growth4,5, it is still challenging to obtain phase-controlled 2D structures6-8. Here we demonstrate an effective synthesis strategy via the progressive transformation of non-van der Waals (non-vdW) solids to 2D vdW transition-metal chalcogenide layers with identified 2H (trigonal prismatic)/1T (octahedral) phases. The transformation, achieved by exposing non-vdW solids to chalcogen vapours, can be controlled using the enthalpies and vapour pressures of the reaction products. Heteroatom-substituted (such as yttrium and phosphorus) transition-metal chalcogenides can also be synthesized in this way, thus enabling a generic synthesis approach to engineering phase-selected 2D transition-metal chalcogenide structures with good stability at high temperatures (up to 1,373 kelvin) and achieving high-throughput production of monolayers. We anticipate that these 2D transition-metal chalcogenides will have broad applications for electronics, catalysis and energy storage.

10.
Int J Paediatr Dent ; 30(2): 110-117, 2020 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-31650633

RESUMO

The International Associations for Dental Research (IADR) annual meeting is one of the most important dental meetings throughout the world, and researches about paediatric dentistry presented in this platform are often used to guide clinical work. To evaluate the publication outcomes of oral and poster paediatric proceedings, which were accepted by the International Associations for Dental Research (IADR), annual meetings from 2010 to 2016 and to analyse the possible factors influencing an abstract's progression to publication. Oral and poster abstracts were retrieved from the official website of IADR (2010-2016). Searching for subsequent publications was conducted in PubMed and Google Scholar (up to March 2019). Two authors independently selected studies, collected, and analysed data. A total of 1396 abstracts were identified, including 275 oral presentations and 1121 poster presentations. Finally, 606 were published in peer-reviewed journals, with a publication rate of 43.41%. Abstracts were published earlier if it is from Europe, well funded, presented orally, or with large sample size. The high publication rate of the IADR proceedings supported the impact of IADR annual meetings on paediatric dentistry in the last 10 years.


Assuntos
Pesquisa em Odontologia , Publicações , Indexação e Redação de Resumos , Criança , Congressos como Assunto , Humanos , Odontopediatria , Sociedades Médicas
11.
ACS Nano ; 14(1): 767-776, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31834778

RESUMO

Large-scale implementation of electrochemical water splitting for hydrogen evolution requires cheap and efficient catalysts to replace expensive platinum. However, catalysts that work well at high current densities with ultrafast intrinsic activities is still the central challenge for hydrogen evolution. An ideal case is to use single atoms on monolayer two-dimensional (2D) materials, which simplifies the system and in turn benefits the mechanism study, but is a grand challenge to synthesize. Here, we report a universal cold hydrogen plasma reduction method for synthesizing different single atoms sitting on 2D monolayers. In the case of molybdenum disulfide, we design and identify a type of active site, i.e., unsaturated Mo single atoms on cogenetic monolayer molybdenum disulfide. The catalyst shows exceptional intrinsic activity with a Tafel slope of 36.4 mV dec-1 in 0.5 M H2SO4 and superior performance at a high current density of 400 mA cm-2 with an overpotential of ∼260 mV, based on single flake microcell measurements. Theoretical studies indicate that coordinately unsaturated Mo single atoms sitting on molybdenum disulfide increase the bond strength between adsorbed hydrogen atoms and the substrates through hybridization, leading to fast hydrogen adsorption/desorption kinetics and superior hydrogen evolution activity. This work shines fresh light on preparing highly efficient electrocatalysts for water splitting and other electrochemical processes, as well as provides a general method to synthesize single atoms on two-dimensional monolayers.

12.
J Phys Chem Lett ; 10(21): 6551-6557, 2019 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-31597421

RESUMO

Cobalt-nitrogen-functionalized materials have been recognized as promising catalysts for the CO2 reduction reaction because of their superior activity. In order to further improve their activity, we proposed an optimization method through coordination engineering in cobalt-nitrogen-functionalized porphyrin and graphene. By considering a series of derived structures with coordinating nitrogen atoms substituted by carbon or oxygen atoms, a clear activity trend is obtained by constructing a volcano-type plot for activity against adsorption energies of *CO. Detailed electronic structure analysis shows that the enhanced catalytic activity is due to the lacking of π bonding in Co-O bonds compared to Co-C or Co-N bonds in cobalt-centered motifs. This difference allows us to predict the catalytic activity by using the vacancy formation energy of the cobalt atom. Our work provides a general guideline for a rational design of efficient catalysts, which may stimulate further study of coordination engineering for other key energy conversion processes.

13.
Small ; 15(45): e1902789, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31544354

RESUMO

Palladium diselenide (PdSe2 ) is an emerging 2D layered material with anisotropic optical/electrical properties, extra-high carrier mobility, excellent air stability, etc. So far, ultrathin PdSe2 is mainly achieved via mechanical exfoliation from its bulk counterpart, and the direct synthesis is still challenging. Herein, the synthesis of ultrathin 2D PdSe2 on conductive Au foil substrates via a facile chemical vapor deposition route is reported. Intriguingly, an anisotropic growth behavior is detected from the evolution of ribboned flakes with large length/width ratios, which is well explained from the orthorhombic symmetry of PdSe2 . A unique even-layered growth mode from 2 to 20 layers is also confirmed by the perfect combination of onsite scanning tunneling microscopy characterizations, through deliberately scratching the flake edge to expose both even and odd layers. This even-layered, ribboned 2D material is expected to serve as a perfect platform for exploring unique physical properties, and for developing high-performance electronic and optoelectronic devices.

14.
J Am Chem Soc ; 141(47): 18694-18703, 2019 Nov 27.
Artigo em Inglês | MEDLINE | ID: mdl-31558019

RESUMO

Two-dimensional (2D) metallic transition metal dichalcogenides (MTMDCs) have attracted tremendous interest due to their intriguing physical properties and broad application potential. However, batch production of high-quality 2D MTMDCs based on existing synthesis on 2D surfaces remains a huge challenge. Herein, a universal synthetic route for the scalable synthesis of high-quality 2D MTMDC (e.g., TaS2, V5S8, and NbS2) nanosheets using microcrystalline NaCl crystals as templates via a facile chemical vapor deposition method is reported. Obviously, this synthetic route is perfectly compatible with a facile water dissolution-filtration process for obtaining high-purity MTMDC nanosheet powders. Representatively, a thickness-uniform 1T-TaS2 nanosheet product can be achieved that shows unexceptionable dispersibility in ethanol, which allows its assembly onto arbitrary substrates/electrodes for high-performance energy-related applications, herein serving as a high-performance electrocatalyst for the hydrogen evolution reaction. This work sheds light on the batch production, green transfer, and energy-related application of 2D MTMDC materials.

15.
ACS Appl Mater Interfaces ; 11(28): 25547-25555, 2019 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-31273972

RESUMO

Although dislocations and grain boundaries (GBs) are ubiquitous in large-scale MoS2 samples, their interaction with phonons, which plays an important role in determining the lattice thermal conductivity of polycrystalline MoS2, remains elusive. Here, we perform a systematic study of the heat transport in two-dimensional polycrystalline MoS2 by both molecular dynamics simulation and atomic Green's function method. Our results indicate that the thermal boundary conductance of GBs of MoS2 is in the range from 6.4 × 108 to 35.3 × 108 W m-2 K-1, which is closely correlated with the overlap between the vibrational density of states of GBs and those of the pristine lattice, as well as the GB energy. It is found that the GBs strongly scatter the phonons with frequency larger than 2 THz, accompanied by a pronounced phonon localization effect and significantly reduced phonon group velocities. Furthermore, by comparing the results from realistic polycrystalline MoS2 to those from different theoretical models, we observe that the Casimir model is broken down and detailed phonon dynamics at a specific GB should be taken into account to accurately describe the phonon transport in polycrystalline materials. Our findings will provide useful guidelines for designing efficient thermoelectric and thermal management materials based on phonon-GB interaction.

16.
J Phys Chem Lett ; 10(13): 3750-3755, 2019 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-31244272

RESUMO

Because of their earth-abundant, low-cost, and environmentally benign characteristics, two-dimensional (2D) group IV metal chalcogenides (e.g., SnSe2) with layered structures have shown great potential in optoelectronic, photovoltaic, and thermoelectric applications. However, the intrinsic motion of excited carriers and their coupling with lattice photons, which fundamentally dictates device operation and optimization, remain yet to be unraveled. Herein, we directly follow the ultrafast carrier and photon dynamics of colloidal SnSe2 nanosheets in real time using ultrafast transient absorption spectroscopy. We show ∼0.3 ps intervalley relaxation process of photoexcited energetic carriers and ∼3 ps carrier defect trapping process with a long-lived trapped carrier (∼1 ns), highlighting the importance of trapped carriers in optoelectronic devices. In addition, ultrashort laser pulse impulsively drives coherent out-of-plane lattice vibration in SnSe2, indicating strong electron-phonon coupling in SnSe2. This strong electron-phonon coupling could impose a fundamental limit on SnSe2 photovoltaic devices but benefit its thermoelectric applications.

17.
ACS Nano ; 13(7): 8442-8451, 2019 Jul 23.
Artigo em Inglês | MEDLINE | ID: mdl-31241317

RESUMO

Among two-dimensional (2D) transition-metal dichalcogenides (TMDCs), platinum diselenide (PtSe2) stands in a distinct place due to its fancy transition from type-II Dirac semimetal to semiconductor with a thickness variation from bulk to monolayer (1 ML) and the related versatile applications especially in mid-infrared detectors. However, achieving atomically thin PtSe2 is still a challenging issue. Herein, we have designed a facile chemical vapor deposition (CVD) method to achieve the synthesis of atomically thin 1T-PtSe2 on an electrode material of Au foil. Thanks to the high crystalline quality, we have confirmed the complete transition from semimetal to semiconductor from trilayer (3 ML) to 1 ML 1T-PtSe2. More importantly, we have found that such atomically thin 1T-PtSe2 can serve as perfect electrocatalysts, featured with a record high hydrogen evolution reaction (HER) efficiency (comparable to traditional Pt catalyst). Our work is helpful toward the large-scale synthesis, exotic physical property exploration, and intriguing application development of atomically thin TMDCs.

18.
J Am Chem Soc ; 141(23): 9408-9414, 2019 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-31117669

RESUMO

Soft porous crystals (SPCs) that exhibit stimuli-responsive dynamic sorption behavior are attracting interest for gas storage/separation applications. However, the design and synthesis of SPCs is challenging. Herein, we report a new type of SPC based on a [2 + 3] imide-based organic cage (NKPOC-1) and find that it exhibits guest-induced breathing behavior. Various gases were found to induce activated NKPOC-1 crystals to reversibly switch from a "closed" nonporous phase (α) to two porous "open" phases (ß and γ). The net effect is gate-opening behavior induced by CO2 and C3 hydrocarbons. Interestingly, NKPOC-1-α selectively adsorbs propyne over propylene and propane under ambient conditions. Thus, NKPOC-1-α has the potential to separate binary and ternary C3 hydrocarbon mixtures, and the performance was subsequently verified by fixed bed column breakthrough experiments. In addition, molecular dynamics calculations and in situ X-ray diffraction experiments indicate that the gate-opening effect is accompanied by reversible structural transformations. The adsorption energies from molecular dynamics simulations aid are consistent with the experimentally observed selective adsorption phenomena. The understanding gained from this study of NKPOC-1 supports the further development of SPCs for applications in gas separation/storage because SPCs do not inherently suffer from the recyclability problems often encountered with rigid materials.

19.
Small ; 15(27): e1805145, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31111665

RESUMO

Migration of dislocations not only determines the durability of large-scale nanoelectronic and opto-electronic devices based on polycrystalline 2D transition-metal dichalcogenides (TMDCs), but also plays an important role in enhancing the performance of novel memristors. However, a fundamental question of the migration dependence on the electronic effects, which are inevitable in practical field-effect transistors based on 2D TMDCs, and its interplay with different dislocations, remains unexplored. Here, taking WS2 as an example, first-principle calculations are used to show that the electronic contributions arising from defect states can greatly influence the migration barriers of dislocations. The barrier height can be reduced by as much as 50%, which is mainly attributed to the change in electronic occupation and the band energy of defect levels controlled by electronic chemical potential (Fermi level). The reduced barriers in turn lead to significantly enhanced migration, and thus the plasticity. Since defect levels from dislocations locate deep inside the bandgap, the doping-induced tuning of barrier height can be achieved at relatively low doping concentration through either chemical doping or electrode gating. The effective electromechanical coupling in 2D TMDCs can provide new opportunities in material engineering for various potential applications.

20.
Nat Commun ; 10(1): 269, 2019 01 17.
Artigo em Inglês | MEDLINE | ID: mdl-30655511

RESUMO

Large-scale implementation of electrochemical hydrogen production requires several fundamental issues to be solved, including understanding the mechanism and developing inexpensive electrocatalysts that work well at high current densities. Here we address these challenges by exploring the roles of morphology and surface chemistry, and develop inexpensive and efficient electrocatalysts for hydrogen evolution. Three model electrocatalysts are flat platinum foil, molybdenum disulfide microspheres, and molybdenum disulfide microspheres modified by molybdenum carbide nanoparticles. The last catalyst is highly active for hydrogen evolution independent of pH, with low overpotentials of 227 mV in acidic medium and 220 mV in alkaline medium at a high current density of 1000 mA cm-2, because of enhanced transfer of mass (reactants and hydrogen bubbles) and fast reaction kinetics due to surface oxygen groups formed on molybdenum carbide during hydrogen evolution. Our work may guide rational design of electrocatalysts that work well at high current densities.

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