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1.
iScience ; 23(3): 100926, 2020 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-32146324

RESUMO

Long decoherence time is a key consideration for molecular magnets in the application of the quantum computation. Although previous studies have shown that the local symmetry of spin carriers plays a crucial part in the spin-lattice relaxation process, its role in the spin decoherence is still unclear. Herein, two nine-coordinated capped square antiprism neodymium moieties [Nd(CO3)4H2O]5- with slightly different local symmetries, C1 versus C4 (1 and 2), are reported, which feature in the easy-plane magnetic anisotropy as shown by the high-frequency electron paramagnetic resonance (HF-EPR) studies. Detailed analysis of the relaxation time suggests that the phonon bottleneck effect is essential to the magnetic relaxation in the crystalline samples of 1 and 2. The 240 GHz Pulsed EPR studies show that the higher symmetry results in longer decoherence times, which is supported by the first principle calculations.

2.
Chemistry ; 2020 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-32196795

RESUMO

The phosphate cathode materials are practical in sodium-ion batteries (SIBs) owing to their high stability and long-term cycle life. In this work, temperature-dependent properties of phosphate cathode Na 3 V 2 (PO 4 ) 2 O 2 F (abbr. NVPOF) are studied in a wide temperature range of -25 ~ 55°C. As cycling at general temperature (above 0°C), the NVPOF cathode can remain excellent charge-discharge performance, and the rate capability is noteworthy, indicating that NVPOF is a competitive candidate for temperature-adaptive cathode of SIBs. When the temperature decreases below 0°C, the performance of the cell degrades, which may derive from the electrolyte and Na electrode, basing on the study of ionic conductivity and electrode kinetics. It proposes a new breakthrough point for developing the SIBs with high-performance in a wide temperature range for the advanced power systems.

3.
Small ; : e1907645, 2020 Mar 05.
Artigo em Inglês | MEDLINE | ID: mdl-32141157

RESUMO

Polyanion-type phosphate materials are highly promising cathode candidates for next-generation batteries due to their excellent structural stability during cycling; however, their poor conductivity has impeded their development. Isostructural and multivalent anion substitution combined with carbon coating is proposed to greatly improve the electrochemical properties of phosphate cathode in sodium-ion batteries (SIBs). Specifically, multivalent tetrahedral SiO4 4- substitute for PO4 3- in Na3 V2 (PO4 )3 (NVP) lattice, preparing the optimal Na3.1 V2 (PO4 )2.9 (SiO4 )0.1 with high-rate capability (delivering a high capacity of 82.5 mAh g-1 even at 20 C) and outstanding cyclic stability (≈98% capacity retention after 500 cycles at 1 C). Theoretical calculation and experimental analyses reveal that the anion-substituted Na3.1 V2 (PO4 )2.9 (SiO4 )0.1 reduces the bandgap of NVP lattice and enhanced its structural stability, Na+ -diffusion kinetics and electronic conductivity. This strategy of multivalent and isostructural anion substitution chemistry provides a new insight to develop advanced phosphate cathodes.

4.
Chemistry ; 26(4): 853-862, 2020 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-31691394

RESUMO

The Fe-based transition metal oxides are promising anode candidates for lithium storage considering their high specific capacity, low cost, and environmental compatibility. However, the poor electron/ion conductivity and significant volume stress limit their cycle and rate performances. Furthermore, the phenomena of capacity rise and sudden decay for α-Fe2 O3 have appeared in most reports. Here, a uniform micro/nano α-Fe2 O3 nanoaggregate conformably enclosed in an ultrathin N-doped carbon network (denoted as M/N-α-Fe2 O3 @NC) is designed. The M/N porous balls combine the merits of secondary nanoparticles to shorten the Li+ transportation pathways as well as alleviating volume expansion, and primary microballs to stabilize the electrode/electrolyte interface. Furthermore, the ultrathin carbon shell favors fast electron transfer and protects the electrode from electrolyte corrosion. Therefore, the M/N-α-Fe2 O3 @NC electrode delivers an excellent reversible capacity of 901 mA h g-1 with capacity retention up to 94.0 % after 200 cycles at 0.2 A g-1 . Notably, the capacity rise does not happen during cycling. Moreover, the lithium storage mechanism is elucidated by ex situ XRD and HRTEM experiments. It is verified that the reversible phase transformation of α↔γ occurs during the first cycle, whereas only the α-Fe2 O3 phase is reversibly transformed during subsequent cycles. This study offers a simple and scalable strategy for the practical application of high-performance Fe2 O3 electrodes.

5.
Radiology ; 294(1): 19-28, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31746687

RESUMO

Background Deep learning (DL) algorithms are gaining extensive attention for their excellent performance in image recognition tasks. DL models can automatically make a quantitative assessment of complex medical image characteristics and achieve increased accuracy in diagnosis with higher efficiency. Purpose To determine the feasibility of using a DL approach to predict clinically negative axillary lymph node metastasis from US images in patients with primary breast cancer. Materials and Methods A data set of US images in patients with primary breast cancer with clinically negative axillary lymph nodes from Tongji Hospital (974 imaging studies from 2016 to 2018, 756 patients) and an independent test set from Hubei Cancer Hospital (81 imaging studies from 2018 to 2019, 78 patients) were collected. Axillary lymph node status was confirmed with pathologic examination. Three different convolutional neural networks (CNNs) of Inception V3, Inception-ResNet V2, and ResNet-101 architectures were trained on 90% of the Tongji Hospital data set and tested on the remaining 10%, as well as on the independent test set. The performance of the models was compared with that of five radiologists. The models' performance was analyzed in terms of accuracy, sensitivity, specificity, receiver operating characteristic curves, areas under the receiver operating characteristic curve (AUCs), and heat maps. Results The best-performing CNN model, Inception V3, achieved an AUC of 0.89 (95% confidence interval [CI]: 0.83, 0.95) in the prediction of the final clinical diagnosis of axillary lymph node metastasis in the independent test set. The model achieved 85% sensitivity (35 of 41 images; 95% CI: 70%, 94%) and 73% specificity (29 of 40 images; 95% CI: 56%, 85%), and the radiologists achieved 73% sensitivity (30 of 41 images; 95% CI: 57%, 85%; P = .17) and 63% specificity (25 of 40 images; 95% CI: 46%, 77%; P = .34). Conclusion Using US images from patients with primary breast cancer, deep learning models can effectively predict clinically negative axillary lymph node metastasis. Artificial intelligence may provide an early diagnostic strategy for lymph node metastasis in patients with breast cancer with clinically negative lymph nodes. Published under a CC BY 4.0 license. Online supplemental material is available for this article. See also the editorial by Bae in this issue.

6.
ACS Appl Mater Interfaces ; 11(51): 47886-47893, 2019 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-31797668

RESUMO

The intrinsic charge-transfer property bears the primary responsibility for the sluggish redox kinetics of the common electrode materials, especially operated at low temperatures. Herein, we report the crafting of homogeneously confined Fe7Se8 nanoparticles with a well-defined graphitic carbon matrix that demonstrate a highly efficient charge-transfer system in a designed natural coral-like structure (cl-Fe7Se8@C). Notably, the intricate architecture as well as highly conductive peculiarity of C concurrently satisfy the demands of achieving fast ionic/electrical conductivities for both Li/Na-ion batteries in a wide temperature range. For example, when cl-Fe7Se8@C is employed as the anode material to assemble full batteries with the cathode of Na3V2(PO4)2O2F (NVPOF), decent capacities of 323.1 and 175.9 mA h g-1 can be acquired at temperatures of 25 and -25 °C, respectively. This work is significant for further developing potential anode materials for advanced energy storage and conversion under low-temperature conditions.

7.
Chem Sci ; 10(33): 7695-7701, 2019 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-31588317

RESUMO

Two homologous covalent triazine frameworks (CTFs) have been developed for the first time as anode materials for high performance K-ion batteries (KIBs). The two-dimensional sheet-like structure as well as the regular channels in CTFs enable the process of intercalation/deintercalation of K-ions into/from the CTF interlayers reversibly. Particularly, a size effect of the porous structure is found to dominate the K-ion storage behavior. CTF-0 with a smaller pore size displays a higher K-ion storage capacity than CTF-1. Molecular simulations reveal the operation mechanism, showing that the depotassiation process in CTF-0 is exothermic while the depotassiation in CTF-1 is endothermic, which makes the deintercalation of K-ions from CTF-0 more feasible than from CTF-1 and contributes to the higher reversible capacity of CTF-0. This work provides a promising strategy for rational design of high-performance organic anode materials by structural modulation at the molecular scale.

8.
Chemistry ; 25(66): 15173-15181, 2019 Nov 27.
Artigo em Inglês | MEDLINE | ID: mdl-31544301

RESUMO

Owing to low ion/electron conductivity and large volume change, transitional metal dichalcogenides (TMDs) suffer from inferior cycle stability and rate capability when used as the anode of lithium-ion batteries (LIBs). To overcome these disadvantages, amorphous molybdenum sulfide (MoSx ) nanospheres were prepared and coated with an ultrathin carbon layer through a simple one-pot reaction. Combining X-ray photoelectron spectroscopy (XPS) with theoretical calculations, MoSx was confirmed as having a special chain molecular structure with two forms of S bonding (S2- and S2 2- ), the optimal adsorption sites of Li+ were located at S2 2- . As a result, the MoSx electrode exhibits superior cycle and rate capacities compared with crystalline 2H-MoS2 (e.g., delivering a high capacity of 612.4 mAh g-1 after 500 cycles at 1 A g-1 ). This is mainly attributed to more exposed active S2 2- sites for Li storage, more Li+ transfer pathways for improved ion conductivity, and suppressed electrode structure pulverization of MoSx derived from the inherent chain-like molecular structure. Quantitative charge storage analysis further demonstrates the improved pseudocapacitive contribution of amorphous MoSx induced by fast reaction kinetics. Moreover, the morphology contrast after cycling demonstrates the dispersion of active materials is more uniform for MoSx than 2H-MoS2 , suggesting the MoSx can well accommodate the volume stress of the electrode during discharging. Through regulating the molecular structure, this work provides an effective targeted strategy to overcome the intrinsic issues of TMDs for high-performance LIBs.

9.
Small ; 15(40): e1902491, 2019 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-31379137

RESUMO

Lithium-sulfur (Li-S) batteries have been disclosed as one of the most promising energy storage systems. However, the low utilization of sulfur, the detrimental shuttling behavior of polysulfides, and the sluggish kinetics in electrochemical processes, severely impede their application. Herein, 3D hierarchical nitrogen-doped carbon nanosheets/molybdenum phosphide nanocrystal hollow nanospheres (MoP@C/N HCSs) are introduced to Li-S batteries via decorating commercial separators to inhibit polysulfides diffusion. It acts not only as a polysulfides immobilizer to provide strong physical trapping and chemical anchoring toward polysulfides, but also as an electrocatalyst to accelerate the kinetics of the polysulfides redox reaction, and to lower the Li2 S nucleation/dissolution interfacial energy barrier and self-discharge capacity loss in working Li-S batteries, simultaneously. As a result, the Li-S batteries with MoP@C/N HCS-modified separators show superior rate capability (920 mAh g-1 at 2 C) and stable cycling life with only 0.04% capacity decay per cycle over 500 cycles at 1 C with nearly 100% Coulombic efficiency. Furthermore, the Li-S battery can achieve a high area capacity of 5.1 mAh cm-2 with satisfied capacity retention when the cathode loading reaches 5.5 mg cm-2 . This work offers a brand new guidance for rational separator design into the energy chemistry of high-stable Li-S batteries.

10.
Adv Mater ; 31(40): e1903125, 2019 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-31402540

RESUMO

Hard carbon is regarded as a promising anode material for sodium-ion batteries (SIBs). However, it usually suffers from the issues of low initial Coulombic efficiency (ICE) and poor rate performance, severely hindering its practical application. Herein, a flexible, self-supporting, and scalable hard carbon paper (HCP) derived from scalable and renewable tissue is rationally designed and prepared as practical additive-free anode for room/low-temperature SIBs with high ICE. In ether electrolyte, such HCP achieves an ICE of up to 91.2% with superior high-rate capability, ultralong cycle life (e.g., 93% capacity retention over 1000 cycles at 200 mA g-1 ) and outstanding low-temperature performance. Working mechanism analyses reveal that the plateau region is the rate-determining step for HCP with a lower electrochemical reaction kinetics, which can be significantly improved in ether electrolyte.

11.
Nanoscale ; 11(35): 16690, 2019 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-31465062

RESUMO

Correction for 'Ionic-liquid-bifunctional wrapping of ultrafine SnO2 nanocrystals into N-doped graphene networks: high pseudocapacitive sodium storage and high-performance sodium-ion full cells' by Yan Yang et al., Nanoscale, 2019, 11, 14616-14624.

12.
Chem Commun (Camb) ; 55(58): 8406-8409, 2019 Jul 25.
Artigo em Inglês | MEDLINE | ID: mdl-31257383

RESUMO

Metallic lithium protection plays a crucial role on improving the electrochemical properties of Li-anode-based batteries. Herein, for an advanced Li//graphite dual-ion battery, constructing a robust and conductive film of carbon nanofibers on a Li anode effectively achieves dendrite-free Li growth and hence significantly enhances the long-life cyclic stability.

13.
Nanoscale ; 11(31): 14959-14960, 2019 08 08.
Artigo em Inglês | MEDLINE | ID: mdl-31353391

RESUMO

Correction for 'Ionic-liquid-bifunctional wrapping of ultrafine SnO2 nanocrystals into N-doped graphene networks: high pseudocapacitive sodium storage and high-performance sodium-ion full cells' by Yan Yang et al., Nanoscale, 2019, DOI: 10.1039/c9nr02542a.

14.
Nanoscale ; 11(31): 14616-14624, 2019 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-31259336

RESUMO

Sodium ion batteries are in great need of electrode materials with high specificity and rate capability being developed. The sluggish reaction kinetics of SnO2-based materials has impeded their applications as anodes of SIBs. Designing electrode materials with high pseudocapacitive contribution can increase the near-surface faradaic reaction, which helps to improve their kinetics and achieve high rate capability. Here, we designed a high-pseudocapacitance sodium storage anode SnO2/N-rGO by downsizing the particle size of SnO2 and constructing an N-doped graphene wrapped structure. The ultrafine structure of SnO2 ensures the high faradaic near-surface reaction, while the N-doped graphene matrix guarantees the superior electron and Na+ diffusion. Meanwhile, the wrapped N-doped graphene acts as a buffer layer to alleviate the volumetric changes of the active SnO2. The obtained ultrafine SnO2/N-graphene composite exhibits a high capacity of 607.6 mA h g-1 at 50 mA g-1 with an impressive rate capability (261.8 mA h g-1 at 2 A g-1) in Na+ half-cells. Furthermore, a good performance with a capacity of 133.3 mA h g-1 at 2.4 A g-1 in Na+ full-cells can also be achieved, which makes it a promising anode material for SIBs.

15.
ACS Appl Mater Interfaces ; 11(27): 24192-24197, 2019 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-31188554

RESUMO

Na super ionic conductor (NASICON)-structured materials have evolved to play many critical roles in battery systems because of their three-dimensional framework structures. Here, by coupling NASICON-structured Na3V2(PO4)2O2F cathodes and Na3V2(PO4)3 anodes, an asymmetric Na-ion-based full cell exhibits two flat voltage plateaus at about 2.3 and 1.9 V and a high capacity of 101 mA h/g. Moreover, an all-solid-state Na-ion battery has been further enabled by the concept of using all NASICON-structured materials, including cathodes, anodes, and electrolytes (Na5YSi4O12), which delivers a high output voltage. Importantly, the full cell displays high safety without using a flammable organic liquid electrolyte and superior structure stability with all NASICON-structured materials.

16.
Chemistry ; 25(38): 8975-8981, 2019 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-31021424

RESUMO

Lithium-ion batteries (LIBs) are one of the most significant energy storage devices applied in power supply facilities. However, a huge number of spent LIBs would bring harmful resource waste and environmental hazards. In this study, a benign hydrometallurgical method using phytic acid as precipitant is proposed to recover useful metallic Mn ions from spent LiMn2 O4 batteries. Besides Mn-based cathodes, this recovery process is also applicable for other commercial batteries. More importantly, for the first time, the as-obtained manganous complex is employed as a nanofiller in a polyethylene oxide matrix to largely improve Li+ conductivity and transference number. As a result, when applied in all-solid-state lithium batteries, high capacity and outstanding cyclic stability are achieved with capacity retention of 86.4 % after 60 cycles at 0.1 C. The recovery of spent lithium batteries not only has benefits for the environment and resources, but also shows great potential application in all-solid-state lithium batteries, which opens up a costless and efficient circulation pathway for clean and reliable energy storage systems.

17.
Nanotechnology ; 30(21): 214002, 2019 May 24.
Artigo em Inglês | MEDLINE | ID: mdl-30865590

RESUMO

An advanced hierarchically porous nanosheets-constructed three-dimensional (3D) carbon material (HPNSC) is prepared by using low-cost agricultural waste-nelumbium seed-pods as the precursor, and potassium hydroxide (KOH) as the activator. The as-prepared HPNSC material has a hierarchically porous nanosheets-constructed structure with 3D carbon nanosheet network morphology, which can enable fast and efficient transfer of Li+/Na+/H+ during charge-discharge process. The assembled HPNSC//HPNSC symmetric supercapacitors exhibit an improved energy density of 41.3 W h kg-1 with a power density of 180 W kg-1 in 1 mol l-1 Na2SO4 electrolyte. The energy density can still be maintained at 16.3 W h kg-1 even if the power density is increased to 9000 W kg-1. When acting as the reversible electrode for lithium ion batteries, this HPNSC material can achieve a high specific capacity of 1246 mA h g-1 at 0.1 A g-1. Moreover, sodium ion battery with HPNSC electrode exhibits excellent cycling performance of 161.8 mA h g-1 maintained even after being cycled 3350 times. The electrochemical performances clearly indicate that the HPNSC developed in this work is a very promising energy storage electrode material, and can further provide new insights for designing and developing highly porous materials for energy storage in other fields.

18.
World J Gastroenterol ; 25(6): 672-682, 2019 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-30783371

RESUMO

Artificial intelligence (AI), particularly deep learning algorithms, is gaining extensive attention for its excellent performance in image-recognition tasks. They can automatically make a quantitative assessment of complex medical image characteristics and achieve an increased accuracy for diagnosis with higher efficiency. AI is widely used and getting increasingly popular in the medical imaging of the liver, including radiology, ultrasound, and nuclear medicine. AI can assist physicians to make more accurate and reproductive imaging diagnosis and also reduce the physicians' workload. This article illustrates basic technical knowledge about AI, including traditional machine learning and deep learning algorithms, especially convolutional neural networks, and their clinical application in the medical imaging of liver diseases, such as detecting and evaluating focal liver lesions, facilitating treatment, and predicting liver treatment response. We conclude that machine-assisted medical services will be a promising solution for future liver medical care. Lastly, we discuss the challenges and future directions of clinical application of deep learning techniques.


Assuntos
Inteligência Artificial , Diagnóstico por Imagem/métodos , Hepatopatias/diagnóstico por imagem , Fígado/diagnóstico por imagem , Algoritmos , Aprendizado Profundo , Humanos , Aprendizado de Máquina
19.
Nanoscale ; 11(3): 1304-1312, 2019 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-30603754

RESUMO

In order to develop promising anode materials for lithium-ion batteries (LIBs), a unique nanocomposite abbreviated as G⊥FP@C-NA, in which a carbon-coated FeP nanorod array (FP@C-NA) is vertically grown on a conductive reduced graphene oxide (G) network, has been successfully prepared via a scalable strategy. Benefiting from the distinctive structure, G⊥FP@C-NA exhibits much improved conductivity, structural stability and pseudocapacitance-boosted ultrafast electrochemical kinetics for Li storage. As a result, the G⊥FP@C-NA delivers a high Li-storage capacity (1106 mA h g-1 at 50 mA g-1), outstanding rate capability (565 mA h g-1 at 5000 mA g-1) and long-term cycling stability (1009 mA h g-1 at 500 mA g-1 after 500 cycles and 310 mA h g-1 at 2000 mA g-1 after 2000 cycles) when used as an anode material for LIBs. As expected, this kind of nanoarray structure is attractive and can also be extended to other electrode materials for various energy storage systems.

20.
Adv Mater ; 31(4): e1804766, 2019 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-30489656

RESUMO

Conventional ion batteries utilizing metallic ions as the single charge carriers are limited by the insufficient abundance of metal resources. Although supercapacitors apply both cations and anions to store energy through absorption and/or Faradic reactions occurring at the interfaces of the electrode/electrolyte, the inherent low energy density hinders its application. The graphite-cathode-based dual-ion battery possesses a higher energy density due to its high working potential of nearly 5 V. However, such a battery configuration suffers from severe electrolyte decomposition and exfoliation of the graphite cathode, rendering an inferior cycle life. Herein, a new surface-modification strategy is developed to protect the graphite cathode from the anion salvation effect and the deposition derived from electrolyte decomposition by generating an artificial solid electrolyte interphase (SEI). Such SEI-modified graphite exhibits superior cycling stability with 96% capacity retention after 500 cycles under 200 mA g-1 at the upper cutoff voltage of 5.0 V, which is much improved compared with the pristine graphite electrode. Through several ex situ studies, it is revealed that the artificial SEI greatly stabilizes the interfaces of the electrode/electrolyte after reconstruction and gradual establishment of the optimal anion-transport path. The findings shed light on a new avenue toward promoting the performance of the dual-ion battery (DIB) and hence to make it practical finally.

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